Alcaraz took just under an hour and 40 minutes to overcome his fellow Spaniard and friend 6-3 6-4, getting 67 per cent of his first serves in and winning 77 per cent of those.
Carreno-Busta struggled to keep the US Open champion at bay, facing 12 break points in all, and although he saved nine of them, his defiance was ultimately in vain.
"It is difficult to play against a friend like Pablo," Alcaraz said on-court after his win on Friday. "Every day we go and have dinner, lunch, together. Every week and we train together, so it is difficult to play against him.
"I also support him and want him to win every match. On court, there are no friends. You have to be focused and go for the match and that is what I did."
Alcaraz will face third seed Felix Auger-Aliassime in the final four after the Canadian defeated Alexander Bublik 6-2 6-3.
The other semi-final will see Roberto Bautista Agut play Holger Rune after the Spaniard beat Stan Wawrinka 7-5 7-6 (7-5) and the Danish teenager defeated Arthur Rinderknech 7-6 (7-0) 6-2.
In Austria, top seed at the Vienna Open Daniil Medvedev beat Jannik Sinner 6-4 6-2 to advance to the last four, where he will play Grigor Dimitrov after the Bulgarian overcame Marcos Giron 6-3 4-6 6-4.
The winner of that contest will face either Denis Shapovalov, who beat Dan Evans 6-3 6-3, or Borna Coric after the Croatian came through against Hubert Hurkacz 6-4 6-7 (2-7) 7-6 (7-5).
The combustible Russian was trailing 6-5 in the third against Alexander Bublik when he appeared to say something to the line judge.
ATP supervisor Roland Herfel came down to the court accompanied by a Russian speaker, who claimed Rublev had sworn in his native language.
Rublev protested, insisting he was speaking in English, while Bublik also backed his opponent.
“I didn’t say ‘f******’. I swear to God. This is huge. I swear to God,” said Rublev.
The offence would usually merit a warning in the first instance, but the 26-year-old was defaulted by umpire Miriam Bley amid jeers from the crowd in Dubai.
It was a controversial end to a tight match, with Kazakhstan’s Bublik progressing to the final 6-7 (4) 7-6 (5) 6-5.
The Italian sixth seed had to fight from 2-5 down in the second set and saved three set points, before powering through to triumph 6-4 7-5 over Lloyd Harris.
"I got a little bit nervous," Berrettini said post-match. “I didn’t like how I handled the start of the second set. I let the anger get out a little bit, which helped. I found the right balance in order to break him in the important moment and then I had the momentum.”
The world number six found another level in reeling off five straight games, and will now face unseeded Miomir Kecmanovic, who accounted for Botic van de Zandschulp 7-6(6-3) 7-5.
Taylor Fritz was also pushed by Spanish qualifier Jaume Munar, taking a third-set tiebreaker to progress to the fourth round.
The 20th-seeded was made to work for it in a match that lasted just under three hours, but Munar feel short in the clutch, with two unforced forehand errors in the closing tiebreak to give Fritz a three-point gap.
In Tuesday's last game, Andrey Rublev showed rare composure to progress past Frances Tiafoe 6-3 6-4.
Neither got off to the best of starts, with Rublev and Tiafoe sharing service breaks in the opening four games of the first set. The characteristically volatile Rublev managed to regroup, though, and stayed calm even when Tiafoe got his home crowd on side.
Despite a low 67 percent on first serve, Rublev won 83 percent of those points, while Tiafoe did himself no favours with an even lower 58 percent first-serve rate.
Last-year’s semi-finalist will face 29th-seeded Alex de Minaur, who defeated Tommy Paul 7-6(6-2) 6-4.
The Australian world no. 31 faced immediate difficulty on service, with only his second service game going to eight consecutive deuces, after five saved break points. He eventually saw the match through, after breaking for 4-3 in the second set.
Fellow seeds Hubert Hurkacz and Grigor Dimitrov both went through relatively unscathed, with respective wins over Steve Johnson and Alexander Bublik.
Dimitrov will face John Isner, who saw past Diego Schwartzman 7-5 6-3 in Tuesday’s other result.
The 24-year-old went into Sunday's match without a career win over a top-five opponent and having lost two finals in a career-best season in 2021.
He was not to be denied this time, however, powering his way to a 6-4 6-3 win over the world number three in Montpellier in just one hour and 10 minutes.
The Kazakhstani lost just four points behind his first serve throughout the match, the only blip coming when he handed Zverev a break back to love after moving 3-2 ahead in the first set.
After regaining the advantage, Bublik survived two more break points before closing out the opener and the pressure only increased on the Zverev serve in the second set.
Bublik broke to love to lead 3-2 and again in the final game as Zverev's resistance wilted.
He can now look forward to rising to a career-high place in the rankings when the updated list is published on Monday.
World number 16 Carreno Busta, the seventh seed at the ATP 500 event in the Netherlands, took the first set with ease but fell to a 2-6 7-6 (7-2) 6-2 defeat against Frenchman Gasquet.
Veteran Gasquet, ranked 45th in the world, will next meet Stan Wawrinka after the Swiss overcame Alexander Bublik in dominant fashion with a 7-6 (7-5) 6-4 triumph.
Grigor Dimitrov recorded a 6-1 6-3 victory over Aslan Karatsev in just 59 minutes to set up a potential second-round tie with fifth seed Hubert Hurkacz, who must first get past Roberto Bautista Agut.
Qualifier Gregoire Barrere was another straight-sets winner, defeating David Goffin 6-0 7-6 (7-3).
The Frenchman, who is ranked 71st in the world, could meet third seed Felix Auger-Aliassime in the next round if the Canadian overcomes Italy's Lorenzo Sonego.
When he trailed by a set and 3-0, Cressy's hopes looked almost forlorn, yet the French-American came back to win 2-6 6-3 7-6 (7-3) in two hours and 23 minutes.
The run of six consecutive games in the second set saved Cressy's skin, before he edged a decider against Russian-born Kazakh rival Bublik in which neither man could force a break of serve.
Cressy had a brief injury timeout near the end of the third set, before sweeping through the tie-break.
The grass-court tournament in Newport, Rhode Island, earlier saw Lleyton Hewitt inaugurated to the International Tennis Federation's Hall of Fame, with the former US Open and Wimbledon champion on hand to receive the accolade.
Hewitt won the last ATP title of his career at the Hall of Fame Open in 2014, having lost in the final in the previous two seasons.
The 41-year-old Australian described the Hall of Fame entry on Sunday as "an incredible honour", saying he had previously considered it out of his reach and "for the people that were my idols growing up and the absolute legends of the sport".
Rafael Nadal's shock defeat to Cameron Norrie – coupled with Katie Swan's win against Nuria Parrizas-Diaz – put Spain 2-0 down in the best-of-five tie ahead of Sunday's action.
World number 13 Paula Badosa put them back into contention with a hard-fought 6-7 (6-8) 7-6 (7-5) 6-1 win against Harriet Dart, but Evans gave Britain an unassailable lead by battling past Ramos-Vinolas, recovering from a dismal second set.
Having topped Group D, Britain will face the Croup C winners – the United States, Germany or the Czech Republic – for a semi-final place on Wednesday.
Meanwhile, Hubert Hurkacz doubled up to help Poland past Kazakhstan, teaming up with Iga Swiatek in the mixed doubles after beating Alexander Bublik.
Hurkacz beat Bublik 7-6 (8-6) 4-6 6-3 in just over two hours before Magda Linette overcame Zhibek Kulambayeva 6-2 6-1.
With Poland's first win in the competition secure, world number one Swiatek helped Hurkacz put the icing on the cake with a 6-3 6-4 victory against Kulambayeva and Grigoriy Lomakin.
The Czech Republic also enjoyed a fruitful day as two-time Wimbledon champion Petra Kvitova downed Laura Siegemund in straight sets to seal the team's win against Germany, but Casper Ruud was less fortunate, with Norway losing their tie against Brazil despite his success against Thiago Monteiro.
The Belgian lost both matches at the inaugural United Cup last week, but he saw off Bublik 6-3 6-4 in 74 minutes to reach the last 16 in New Zealand.
Another seeded player fell at the first hurdle on Monday as Adrian Mannarino lost 6-4 7-6 (7-4) to J.J. Wolf.
Richard Gasquet advanced with a 6-3 6-1 win over wild card Kiranpal Pannu, while Jenson Brooksby beat Fabio Fognini 6-7 (2-7) 6-1 6-3 and will now face Diego Schwartzman.
At the Adelaide International 2, fifth seed Dan Evans suffered a 7-5 7-5 defeat to Mackenzie McDonald.
Fellow seeds Alejandro Davidovich Fokina and Miomir Kecmanovic overcame Brandon Nakashima and Kyle Edmund respectively.
Top seed Hurkacz defeated German qualifier Peter Gojowczyk 6-4 7-6 (7-4) to stand on the brink of a third title of the year.
The world number 13 from Poland won 79 per cent of the points on his first serve and sealed victory in an hour and 37 minutes.
Gojowczyk saved five break points but was unable to pull off an upset in Metz.
Hurkacz said: "Peter played a really great match. He was super tough to play against, so I am proud of myself that I managed my emotions and played a good tie-breaker.
"I was trying to keep holding serve to stay in the second set and ended up taking the set in the tie-breaker."
Carreno Busta ended Gael Monfils' bid to win the title on home soil, the Spaniard triumphing 7-5 7-6 (10-8).
Monfils was 5-3 up in a second-set tie-break but failed to force a decider as Carreno Busta advanced for a showdown with Hurkacz.
James Duckworth is into his first ATP Tour final after beating eighth seed Ilya Ivashka 6-3 7-6 (7-4) at the Astana Open.
The Australian will face Kwon Soon-woo, who upset second seed Alexander Bublik 3-6 7-5 6-3.
The 37-year-old was taking on Kazakhstan's Alexander Bublik and trailed 2-1 in the opening set when he decided he would be unable to complete the match.
Bublik had broken serve and led 40-30 in the fourth game when Wawrinka approached the net and told the umpire he had to stop.
Wawrinka has been battling a thigh injury that appeared to be the cause of his withdrawal, meaning the three-time grand slam champion, now ranked a lowly 284th, could not push on with his quest for a first ATP Tour title in five years. His most recent semi-final appearance, prior to this run in Metz, had come in Doha at the start of 2020.
Italy's Lorenzo Sonego awaits Bublik in Sunday's final after he sank the hopes of Polish second seed Hubert Hurkacz in the first semi-final.
Unseeded Sonego took the win 7-6 (7-5) 6-4 and will be chasing a third ATP title, after previous triumphs in Antalya in 2019 and Cagliari last year.
Bublik, the seventh seed this week, has just one previous singles title, earning that success in February of this year in Montpellier.
The British number four saw off the eccentric Kazakh 7-6 (2) 6-4 to go one better than last year when he fell in the last four.
It represents a second straight ATP Tour final for the 22-year-old, who was beaten by Adrian Mannarino in the trophy decider at the Sofia Open in November.
Draper was twice a break up in the opening set against Bublik, who is one of the most unconventional players on tour.
He dragged Draper around the court with repeated drop shots and one game in the second set featured a rally where both players played lobs between their legs before Bublik sent over an underarm serve and won the point with a volley played with his racket handle.
But there were also nine double faults and a host of unforced errors and Draper maintained his high level to set up a final meeting with Czech Jiri Lehecka.
“It was a really tricky match,” said Draper. “Alexander’s a great player and someone who’s a very unorthodox player. It’s always tricky to play against him.
“He’s actually a really good guy and a good friend as well. We have a lot of fun when we’re competing against each other. I was really happy that I was able to come through and get the win today and be in another final.”
Victory for Draper on Saturday would elevate his ranking back into the top 50 ahead of his Australian Open opener next week.
Kyrgios suffered a disappointing semi-final defeat to Andy Murray in Stuttgart last week, but looked greatly improved against Tsitsipas as he recovered from a set down to win 5-7 6-2 6-4.
It was the second serve of both men where Kyrgios shone, winning 76 per cent (28 of 37) of points on his second serve, and 58 per cent (23 of 40) on his opponent's.
"Stef is one of the best players in the world at the moment and he's going to have some amazing results and I'm sure many, many grand slams," Kyrgios said following his win.
"I don't know if I can say the same for me, but I'm happy to still be able to produce this level with the tournaments I play. It is a testament to how hard I do work when I'm not playing."
He will face Pablo Carreno Busta in the quarter-finals after the Spanish sixth seed beat Sebastian Korda 6-4 0-6 6-3.
Elsewhere, Hubert Hurkacz will face Felix Auger-Aliassime in the last eight after defeating Ugo Humbert 7-6 (7-5) 6-3, while the Canadian also won in straight sets against Mackenzie McDonald 7-6 (9-7) 6-1.
The one remaining first round match saw number one seed Daniil Medvedev beat David Goffin 6-3 6-2 to set up a second round clash with Ilya Ivashka.
At the Queen's Club Championships, sixth seed Denis Shapovalov was eliminated by Tommy Paul 6-4 2-6 6-4, with the American now scheduled to face Stanislas Wawrinka in the second round.
It means that six of the eight seeds in west London were knocked out in the first round, with Matteo Berrettini and Marin Cilic the only remaining seeds. The latter sealed his place in the quarter-finals on Wednesday with a 7-6 (8-6) 7-5 win over Alexander Bublik.
Cilic will play Finland's Emil Ruusuvuori in the last eight after he beat home favourite Jack Draper 6-2 7-6 (7-2).
The best contest of the day came between Alejandro Davidovich Fokina and Alex de Minaur, with the former coming from behind to win 4-6 6-4 7-5 to set up a quarter-final with Botic van de Zandschulp, who beat Grigor Dimitrov 7-6 (7-5) 6-3.
World number one Medvedev fought back from a set down to defeat Aslan Karatsev 3-6 6-4 6-2 and advance to a quarter-final against fifth seed Roberto Bautista Agut, who was granted a walkover after Nick Kyrgios pulled out with an abdominal issue.
The Russian got just 48 per cent of his first serves in during a blustery opening set before improving to 68 per cent in the second and controlling the decider as Karatsev struggled with injury.
"It was tough to play [in] rhythm. It felt like many points were just whoever managed to put the ball in the court was going to win the point," Medvedev said of the tricky conditions.
"It was not easy but I'm happy to win because that's the most important [thing].
"Last year was amazing. I played great tennis. Hopefully I can do the same this year. I like it here in Mallorca, so hopefully I can stay as long as possible in the tournament."
Alongside Medvedev and Bautista Agut, Stefanos Tsitsipas is the only other seed left in the draw after he overcame Ilya Ivashka 6-4 6-4.
Denis Shapovalov was a 6-4 6-1 loser against Benjamin Bonzi, Pablo Carreno Busta went down 6-3 6-4 to Antoine Bellier and Sebastian Baez's meeting with Daniel Altmaier ended in a 6-2 2-6 6-4 defeat for the Argentine.
At the Eastbourne International, second seed Sinner suffered a 6-3 3-6 6-3 loss to Tommy Paul as he made his return from a knee injury sustained at the French Open.
World number 13 Sinner remains without a grass-court win in his ATP Tour career, while Paul will next face defending champion Alex de Minaur, who overcame Lorenzo Sonego 7-6 (7-3) 6-2 in a repeat of last year's final.
Jack Draper defeated fourth seed Diego Schwartzman 7-5 7-6 (7-3) to advance to the quarter-finals and Cameron Norrie cruised past Brandon Nakashima in straight sets.
There were also wins for Maxime Cressy, Alexander Bublik and Taylor Fritz.
World number four Medvedev fell to a 6-4 6-7 (7-9) 6-3 loss against three-time major winner Wawrinka, who will next meet Mikael Ymer after his straight-sets win over home favourite Gregoire Barrere.
Second seed Hurkacz did not experience such struggles against Thiem as the Pole cruised to a 6-3 6-4 as he served 12 aces in a dominant performance in Metz.
Hurkacz will face Arthur Rinderknech in the next round after the Frenchman battled to a 7-6 (13-11) 6-3 triumph over fifth seed Nikoloz Basilashvili.
Alexander Bublik, the seventh favourite in France, was also made to work for his progress to the quarter-finals, downing Emil Ruusuvuori 6-7 (4-7) 6-4 6-3.
Fourth seed Holger Rune awaits Bublik after Benjamin Bonzi retired due to injury when 6-4 4-1 down against the Dane.
Lorenzo Sonego coasted through his second-round clash to defeat Gilles Simon 7-6 (7-2) 6-4 to tee up a last-eight clash with Sebastian Korda.
Bublik's only career title to date came in Montpellier last year, but he will not defend his crown after losing in three sets to Gregoire Barrere in the first round on Wednesday.
That remarkable 6-4 6-7 (12-14) 7-6 (7-3) reverse represented Bublik's seventh loss in seven singles matches so far this season.
The 25-year-old, who has fallen to 50th in the rankings, has lost nine in a row going back to last year.
Bublik worked hard to stay in Wednesday's match in the second set, fending off three match points in the tie-break, but he could not show the same resilience in the decider as Barrere prevailed.
With the champion out, those hoping to take the title this week found life a little easier elsewhere.
Both Jannik Sinner and Alejandro Davidovich Fokina benefited from walkovers, albeit the Spaniard first had to dig in to level his match against Ugo Humbert, who had taken the opener 6-1.
Bublik and Murray have now beaten each other two times apiece this year after the third seed won 7-5 6-4 in Newport.
The Kazakh overpowered the three-time grand slam champion to move into the last four, winning 80 per cent of his first-serve points and breaking three times.
Murray hit back straight after being broken at the start of the second set, but the former world one trailed 4-3 after failing to hold for a third time and Bublik did not give him another look-in.
Bublik will do battle with Jason Kubler for a place in the final after he defeated fellow Australian James Duckworth 7-5 7-6 (7-3).
Sebastian Baez ended Thiem's encouraging run to the quarter-finals with a 6-2 6-7 (5-7) 6-4 win in Bastad.
Thiem, who has endured an injury nightmare, won his first match 14 months by beating Emil Ruusuvuori in the first round and followed that up by getting the better of Roberto Bautista Agut, but the former US Open champion will go no further.
Argentinian Baez will now come up against Andrey Rublev after the second seed from Russia saw off Laslo Djere 7-5 6-4.
Pablo Carreno Busta blew Diego Schwartzman away in a 6-1 6-0 thrashing, while Francisco Cerundolo got past Aslan Karatsev in straight sets.
Murray, ranked 53rd in the world, could not find his usual return with Lajovic winning 72 per cent of second-serve points, prevailing in one hour and 38 minutes.
The Serbian claimed only his fourth win out of 16 matches on hard courts since the start of last year, holding his nerve after failing to serve out the match at 5-4 in the second set, converting his third match point in the 12th game.
Lajovic hit 21-14 winners, with Murray committing more unforced errors (15-13). The Serbian converted all three break points he generated.
Former world number six Gael Monfils was forced to retire due to a right wrist injury in his clash with French compatriot Ugo Humbert at 3-3.
Monfils, 36, was playing at only his third event since returning to the ATP Tour following seven months out due to injury.
Argentina's Facundo Bagnis defeated Brazilian qualifier Felipe Meligeni Alves 6-3 1-6 6-4, with his reward a second-round clash with last week's Indian Wells Open winner and top seed Carlos Alcaraz.
World number 50 J.J. Wolf beat world number 48 Alexander Bublik 7-5 6-3 in 79 minutes, earning a second-round clash with sixth seed Andrey Rublev.
World number 74 Martin Fucsovics sent down nine aces as he beat Argentina's Pedro Cachin 6-4 7-6 (7-2) in 107 minutes. Fucsovics will next face seventh seed Holger Rune.
Ilya Ivashka beat Daniel Altmaier 6-2 6-1 to book a second-round clash with third seed Casper Ruud, while Fabio Fognini bowed out, losing 6-4 5-7 6-4 to Jan-Lennard Struff. USA's Brandon Nakashima powered to a 7-6 (7-3) 6-3 victory over Germany's Oscar Otte.
Murray appeared to be on course for a routine win after taking the first set 6-0, but was broken early in the second, eventually losing 6-3 to take him to a fourth three-set contest in four matches this week in Doha.
Lehecka should have won a hard-fought decider when 5-4 and 40-0 up on his own serve, but Murray's trademark resilience saw him break back despite facing five match points against, before ultimately winning the tie-break 8-6.
"I don't know how I managed to turn that match around," Murray said after the win. "In the 5-4 game, I think I played most of the match points really well. He missed one bad shot on the deuce point in that game at 5-4, but I played the match points pretty well.
"It's been an amazing start to the year. I have never experienced this in my whole career, like this many matches... It was sort of looking [like it might be a quicker match] for 30 minutes and then it turned into something completely different. Yeah, just amazing that I managed to turn that around."
Murray equalled Jimmy Connors for the fifth-most ATP hard court wins in the Open Era (489), and will play Medvedev in the final after the Russian's 6-4 7-6 (9-7) win against Felix Auger-Aliassime.
The Canadian had three set points in the second set tie-break to try and force a decider, but Medvedev showed determination to turn it around and seal his place against Murray in the final.
At the Open 13 Provence, number one seed Hubert Hurkacz is through to face Alexander Bublik in the semi-finals, with both also having to come through three-set matches in a deciding tie-break.
Hurkacz was finally able to overcome Mikael Ymer 6-3 3-6 7-6 (8-6) before Bublik defeated Grigor Dimitrov 7-5 3-6 7-6 (8-6).
Third seed Alex de Minaur was shocked by Benjamin Bonzi, who broke the world number 23 four times on his way to a 6-2 6-4 victory to avenge his third-round defeat at the Australian Open.
Bonzi will meet qualifier Arthur Fils in the final four after the French 18-year-old beat former world number three Stan Wawrinka 6-2 6-3 to reach a second straight tour-level semi-final.
Former world number one Murray secured an impressive 7-6 (8-6) 6-4 victory over Alexander Bublik, who entered the tournament on the back of the biggest win of his career over Alexander Zverev in the Montpellier final last week.
Murray stopped the Kazakh serving out the opening set with a crucial break and appeared in fine form as he closed out the win.
"There were some tough moments in the first set for both of us. I just managed to come through at the end of it. Some great returns off some big second serves from him at the end and I did a good job," said Murray.
"It’s not easy playing against someone like that, huge serves, a lot of drop shots and you’ve got to keep your focus and I did that well."
Up next for Murray is Australian Open quarter-finalist and third seed Auger-Aliassime, who came from a set down to beat qualifier Egor Gerasimov 3-6 6-2 6-2.
"[Auger-Aliassime] started the year pretty well and is one of the best young players just now," said Murray. "I'll need to be on my game if I want to beat him, but it's a great test for me and we'll see what happens out there."
Musetti advanced to the quarter-finals after a 6-3 5-7 6-4 triumph over Hurkacz, dropping just one point on his first serve in the decisive set.
Cameron Norrie defeated Karen Khachanov 6-4 7-6 (7-5) to reach the last eight, while Alex De Minaur was also a 7-6 (8-6) 1-6 6-4 victor against Mackenzie McDonald in the second round.
The former world number one was knocked out of the Hall of Fame Open by Alexander Bublik on Friday, with the Kazakh winning their quarter-final 7-5 6-4 in Newport.
It follows Murray's disappointing second-round exit at Wimbledon to John Isner, and while the 35-year-old wants to see results improve, he was optimistic ahead of the switch from grass to the hard-court season.
"Obviously I just want the results to be a bit better," Murray told the ATP Tour website. "I felt like I had a good chance of [winning] here. If I got through Bublik, it would have been a good opportunity potentially in the semi-finals.
"But… to have my body feeling pretty good and getting lots of matches in is important for me."
Murray did have some success on grass this year, including reaching the final of the Stuttgart Open before losing to Matteo Berrettini.
"There were some good moments, but also some tough ones," he added. "Today's match and the loss at Wimbledon were disappointing and frustrating for me, but then I also had my best wins in a while in Stuttgart.
"So a bit up and down, but a little bit of progress overall and I'll try and keep that going through the hard-court summer.
"[I want] to continue to improve. If I keep seeing progress I’ll continue to keep playing."
Murray met NFL quarterback Kirk Cousins earlier in the week, with the Minnesota Vikings star praising the tennis supremo's "grit", and Murray revealed Cousins was looking to incorporate tennis into his own preparations for the new season.
"I'd never actually met any NFL athletes before, but he seemed like he loved his tennis and he was saying that he feels like a lot of the movements you make in tennis are similar to a quarterback," Murray added.
"He would prefer to do an hour of tennis to an hour of agility drills, which I can understand as you get a little bit older, trying to keep things fresh and fun in training in pre-season is important."