In a contest between two teenage stars, it was 17-year-old Gauff who sealed her second semi-final spot in as many weeks, having made the last four at the Internazionali d'Italia.
Third seed Gauff will face Katerina Siniakova next, after the Czech followed up her win over Serena Williams with a 7-5 6-1 defeat of Caroline Garcia.
"I was pretty satisfied with the way I played," Gauff said, after fending off Anisimova.
"I do think I could have served a little bit better, but other than that, I was pretty happy with the way I played."
Despite her valid concerns, Gauff won 72 per cent of points after landing her first serve and forced six breaks to win in style, reeling off six games on the trot from 3-0 behind in the second set.
The other semi-final will see second seed Wang Qiang take on Sloane Stephens.
Wang prevailed 7-6 (7-4) 3-6 7-5 against Petra Martic, while Stephens saw off Sara Errani 6-3 6-0.
It was another rain-affected day at the Serbia Open, where Maria Camila Osorio Serrano managed to get past Kamilla Rakhimova 4-6 6-3 6-4.
Anna Kalinskaya and Reka Luca Jani were locked at one set apiece in the only other match to get started before the weather halted play.
Gauff joins other big names in exiting the WTA 1000 event, with Naomi Osaka, Garbine Muguruza, Danielle Collins, Paula Badosa and Maria Sakkari among those crashing out in the second round.
The number 14 seed did not put up much resistance against her Romanian opponent, with Halep winning 6-4 6-4 in just 77 minutes.
Gauff struggled on her own serve in particular, making six double faults and only winning 61.5 per cent of her first-serve points, compared to 83.8 from Halep on hers.
The former world number one and two-time Madrid champion will now face the only remaining top-eight seed in the tournament in the quarter-final, Jabeur, who defeated Bencic 6-2 3-6 6-2.
The Tunisian was out for revenge after losing to Bencic at the same stage last year, as well as in the Charleston Open final last month, and took it well as she sealed victory in just over two hours.
"I came here to take my revenge," Jabeur said after the win. "I wish I played like that in the final in Charleston, to be honest.
"Part of me is very proud of myself for coming today and getting the win. Belinda is such an amazing player and it's very tough to play against her. I'm very happy with the level I showed today, and hopefully this level will continue for the rest of the tournament."
Elsewhere, Victoria Azarenka is out after the number 15 seed was beaten 6-1 6-4 by Amanda Anisimova, who will now face Ekaterina Alexandrova in the last eight after she overcame Marie Bouzkova 6-7 (4-7) 6-0 7-5.
Former world number one Halep was the only player to have won the competition to have reached the last eight, but she was no match for the Tunisian, who won 6-3 6-2 in just over an hour.
After a difficult start to the year, Jabeur has hit her stride in recent times and will be contesting a second semi-final in three tournaments.
While Jabeur caught the eye, particularly with her penchant for a dropshot, Halep proved to be her own worst enemy, recording 12 more unforced errors (20) than winners (eight).
Up next for Jabeur is qualifier Ekaterina Alexandrova, who beat 2019 French Open semi-finalist Amanda Anisimova 6-4 6-3 to reach her first WTA 1000 last-four clash.
Alexandrova has won six of her previous seven meetings with Jabeur.
Meanwhile, Anhelina Kalinina saw her impressive run ended by Jil Teichmann. The Ukrainian had seen off three major winners on the bounce in Sloane Stephens, Garbine Muguruza and Emma Raducanu, but she was beaten in straight sets this time.
Teichmann – who won 6-3 6-4 – will face Jessica Pegula for a place in the final, with the American eliminating Spain's final hope of a home winner in Sara Sorribes Tormo, 6-4 6-2.
Linette took just 31 minutes to win the first set in Rome, but world number 10 Kvitova responded superbly to win 1-6 6-0 6-2.
Two-time grand slam champion Kvitova racked up 16 unforced errors in the first set, yet rallied like the great competitor she has proved to be for so long to ensure she will face Vera Zvonareva - conqueror of Christina McHale - in the second round.
The 11th seed from the Czech Republic said: "The first set I started very badly. I was missing almost everything. On the court... [the ball] was bouncing everywhere as well. A little bit windy. I just had to get used to probably everything.
"The beginning of the second set when finally I held my serve and broke her serve, I think since then it was much, much better."
French Open champion Iga Swiatek advanced when Alison Riske retired at 5-4 down in the first set due to a recurrence of a left foot injury.
Swiatek, who will take on Sloane Stephens or Madison Keys in the second round, made 18 unforced errors but had won four games in a row from 4-1 down when the American was unable to continue.
Coco Gauff battled past Yulia Putintseva 7-5 4-6 6-4 to set up a meeting with 17th seed Maria Sakkari - who fended off qualifier Polona Hercog 7-6 (8-6) 3-6 6-2.
Amanda Anisimova will do battle with Elina Svitolina, a winner of this tournament twice, after defeating Wang Qiang 7-5 6-3. Jessie Pegula, Jennifer Brady and Petra Martic were among the other winners on day one.
The 18-year-old Czech was impressive against the third seed as she recorded her first win against anyone in the top 30 of the world rankings.
Fourth seed Veronika Kudermetova eased past Amanda Anisimova in just an hour and 15 minutes, winning 6-3 6-0, while Liudmila Samsonova will face second seed Aryna Sabalenka in the next round after coming from a set down to beat Zhang Shuai 5-7 6-3 6-0.
Irina-Camelia Begu and Elena Rybakina also both came from behind to secure wins, with the latter beating fifth seed Danielle Collins to set up a last-16 clash against Ukrainian Marta Kostyuk, who beat Jaimee Fourlis 6-1 3-6 6-4.
At the ASB Classic in Auckland, 42-year-old Venus Williams comfortably overcame her 21-year-old opponent Katie Volynets 7-6 (7-4) 6-2, and will play China's Zhu Lin next after she eliminated sixth seed Madison Brengle 4-6 7-6 (8-6) 6-4.
Third seed Leylah Fernandez beat Brenda Fruhvirtova 6-1 6-1 to set up a last-16 tie with Julia Grabher after she defeated Tereza Martincova in three sets.
Eighth seed Rebecca Marino is through after beating Dalma Galfi in straight sets and will now face Ysaline Bonaventure, who eventually put away Caty McNally 5-7 6-4 6-4.
Viktoria Kuzmova led fourth seed Bernarda Pera 5-4 in the opening set when rain stopped play for the day.
The incident happened after Osaka had been broken by Kudermetova in the first game, with someone in attendance reported to have yelled "Naomi, you suck".
Four-time grand slam winner Osaka, competing in her first tournament since January's shock early Australian Open exit, appeared to ask the chair umpire to take action.
Osaka initially put that unneeded distraction behind her by taking the next point, but she wasted two break opportunities and Kudermetova successfully held to move 2-0 ahead.
The 24-year-old was in tears as she prepared to serve her next game and held further discussions with the court supervisor after going 3-0 down.
She could not recover and, after losing the first set 6-0, Osaka suffered the only break of serve in the seventh game of the second set to lose the contest fairly resoundingly.
Kudermetova will now face Marie Bouzkova for a place in the last 16 after the Czech recovered to see off home hopeful Jessica Pegula 5-7 6-2 6-0.
Two-time champion Victoria Azarenka also made it through on Saturday with a 6-3 7-5 victory over lucky loser Astra Sharma, setting up a meeting with Elena Rybakina.
Leyla Fernandez saved four match points against Amanda Anisimova in a dramatic match that came to an end when the American retired through illness.
After losing the opener 6-2, Fernandez took the second set to a tie-break but felt unable to continue. Anisimova will meet Shelby Rogers in a rematch of last year's last-16 encounter.
The victory marked Pegula’s second straight Canadian Open title, as she fended off an Anisimova comeback to win 6-3 2-6 6-1.
The 30-year-old, who was seeded third, has become just the seventh player in the Open Era to defend her Canadian Open title, the most recent having been Martina Hingis in 2000.
Pegula, who hails from Buffalo, New York, enjoyed her achievement all the more for the presence of family and friends.
"Toronto, it's nice, it's so close to Buffalo, I had a lot of friends, family, and my grandparents, my husband was able to come today. That's cool, I don't really get that at a lot of tournaments,” said Pegula.
"Then to be able to win the tournament as well, and to be able to share that moment with them is really special.
“I don't know what it is about Canada, but I just seem to do well. Yeah, I'll take it.”
The victory means Pegula has become the first woman to win 10 consecutive singles matches at the Canadian Open since Serena Williams. The 23-time grand slam winner triumphed in 14 straight matches between 2011 and 2014.
"I know everyone's talking about my record, but it's nice to be able to get through the week and to back it up," said Pegula. "So, just super excited, I mean, an honour, really.”
It took Pegula one hour and 27 minutes to defeat Anisimova and win her sixth WTA singles title. It also marked her third career WTA 1000 title (Guadalajara 2022, Montreal 2023 and Toronto 2024).
It was Anisimova's first Tour-level final in over two years, with the 22-year-old having defeated four top-20 players on her way there.
"I put the work in, I kept my head down, and I tried to come back to the sport with more of a relaxed feeling," Anisimova reflected.
"Trying to enjoy each day as it comes and not being so serious about everything, because that takes away the joy from a lot of things. That approach to my everyday life has helped me a lot."
Pegula, who was seeded third, prevailed 6-3 2-6 6-1 against her fellow American in Toronto.
The 30-year-old ended Anisimova's hopes of a shock title, and a fifth top-20 win of the tournament.
Pegula was on fire in the opening set, dominating on her serve, but Anisimova responded with a swift break in the second as she rallied to draw the match.
Yet two breaks in quick succession put Pegula firmly on top in the decider, and though Anisimova clawed back two match points, her opponent got the job done at the third time of asking.
Pegula has now won six Tour-level titles, with three of these being WTA 1000 events (Guadalajara 2022, Montreal 2023 and Toronto 2024).
Data Debrief: Pegula's Canadian comforts
Hailing from Buffalo, just south of the border, Pegula has certainly enjoyed a fine run in Canada over the past two years.
She is only the second player this century to secure the title at the Canadian Open in both Toronto and Montreal, along with Simona Halep, while she became the seventh player in the Open Era to defend her title at the Canadian Open after Chris Evert, Evonne Goolagong, Martina Navratilova, Regina Marsikova, Monica Seles and Martina Hingis.
No player had successfully defended a WTA 1000 title since Iga Swiatek did so at Rome in 2022, and no player had done so on hard court since Ashleigh Barty, who defended her Miami crown in 2021.
The Briton, who won the US Open in 2021, went down 6-3 3-6 6-2 in a genuine tug-of-war against the 31st-ranked Canadian.
Andreescu sent down seven aces for the match, including four in the first set along with 12 winners as she claimed an early lead.
Raducanu responded with greater aggression, securing the crucial break in the eighth game, before serving out to level the contest.
But Andreescu showed composure and quality in the big points in the final set, winning the final four games to round out the victory, sealing a second-round clash with seventh seed Maria Sakkari.
Andreescu finished with 32 winners compared to Raducanu's 20, while the Briton committed 40 unforced errors.
World number 42 Shelby Rogers edged out USA compatriot Sloane Stephens in just under two hours, winning 6-4 3-6 6-2. Rogers will take on second seed Aryna Sabalenka, who is arguably the tournament favourite after top seed Iga Swiatek's withdrawal, in the next round.
Rogers was one of five Americans to progress, including 2020 Australian Open champion Sofia Kenin who defeated Australia's Storm Hunter 6-0 7-6 (7-5).
World number 35 Amanda Anisimova retired down 7-6 (7-5) 5-2 to countrywoman Madison Brengle.
Leylah Fernandez, the player whom Raducanu beat in the 2021 US Open final, advanced into the second round with a 6-4 6-3 victory over Lesia Tsurenko in 88 minutes.
The world number 12 was trailing 6-2 2-1 when calling time on the match against Andreescu in a highly anticipated showdown between two of the past three US Open winners.
Raducanu initially left the court for treatment ahead of the seventh game of the opening set for a medical timeout and completed just four more games.
Speaking after her withdrawal, coming two weeks before the French Open, Raducanu explained she did not want to aggravate an injury sustained at last week's Madrid Open.
"I thought maybe taking one, two days off, it would go away because a lot of the other small niggles I've had, they've kind of gone away after taking, like, two days off," she said.
"Then I got here and I was training, but it just didn't seem to get better. I was training with some limitations. I wasn't moving really.
"I was just playing where I knew where the ball was coming, just staying in one corner. I think I must have underestimated the unpredictability of competition in a match.
"The last few weeks have been really positive. I've learned a lot about myself and my game has definitely improved on this surface but I need to make sure my back is fully right.
"I need to just keep on it. I don't want to play my next match with a feeling of limitation because I think that I learned my lesson from this week, when to push, when not to push."
Ons Jabeur joined Andreescu in the last 32 with a 6-0 7-6 (7-1) victory over Sorana Cirstea to keep her impressive run of form going.
The Tunisian won her first WTA 1000 title in Madrid last week and has now won seven successive main draw matches for the first time in her career
Elsewhere in Tuesday's action, American qualifier Lauren Davis pulled off a shock 6-2 6-3 win against number 11 seed Jelena Ostapenko.
Fellow Americans Jessica Pegula, Madison Brengle and Amanda Anisimova also advanced, beating Liudmila Samsonova, Marta Kostyuk and Tereza Martincova respectively.
Anisimova, who is now the player with the most wins in three sets so far in 2022 with nine, will face Belinda Bencic for a place in the last 16.
Rybakina won the first set comfortably before the Russian hit back for a remarkable turnaround win, 1-6 6-2 6-0 in one hour and 40 minutes.
Seventh seed Kasatkina was the runner-up at last year's Silicon Valley Classic and found her groove to break her Rybakina six times in the second and third sets.
Rybakina sent down three of her four aces for the match in the first set, but Kasatkina adjusted to her serve and won 52.1 per cent return points for the match.
Eighth seed Karolina Pliskova fought back from a slow start to get past Katie Boulter 1-6 7-6 (7-5) 6-3, despite 16 double faults.
American Amanda Anisimova overcame compatriot Ashlyn Krueger 6-2 7-6 (7-5). US pair Madison Keys and Taylor Townsend were also winners.
Third seed Simona Halep and top seed Jessica Pegula were both among the winners in the first round at the Citi Open in Washington DC.
Two-time major winner Halep cruised past Spanish qualifier Cristina Bucsa 6-3 7-5 in one hour and 20 minutes.
Halep, playing her first match since her Wimbledon semi-final loss to Rybakina, fired 19 winners but also 33 unforced errors.
Defending champion Pegula made light work of countrywoman Hailey Baptiste 6-2 6-2 in 73 minutes.
Pegula will face unseeded Australian Daria Saville, who won in three sets over Mirjam Bjorklund, while sixth seed Kaia Kanepi will meet China's Zhu Lin after both won on Monday.
Fifth seed Elise Mertens was a first-round casualty, going down 7-6 (7-4) 6-4 to Ludmilla Samsonova, while Croatian Donna Vekic knocked off seventh seed Mayar Sherif 6-4 6-1.
Six-time major champion Venus Williams played her first singles match in nearly a year but bowed out 4-6 6-1 6-4 to Rebecca Marino.
Two-time Wimbledon champion Kvitova, the 12th favourite in the United Arab Emirates, eased past Italy's Martina Trevisan 6-2 6-1 to make a dominant start.
World number 15 Samsonova was made to work to beat Paula Badosa, winning 6-7 (3-7) 7-6 (7-5) 6-4 to tee up a clash with Qinwen Zheng, who overcame compatriot Zhang Shuai in straight sets.
Samsonova's triumph took three hours and 22 minutes, the longest match of the WTA Tour season thus far, in a thrilling first-round encounter between two top-20 players.
"Playing against Paula is always tough," 14th seed Samsonova said in her on-court interview. "She's doing unbelievable, so I'm really proud that I stayed on the court until the end.
"I think I'm growing match after match, day by day. I know it's a long journey, and I hope to continue like that."
Barbora Krejcikova, the 2021 French Open champion, cruised into the last 32 with a comfortable 6-4 6-2 victory over Irina-Camelia Begu as she aims to go one better than her runners-up finish two years ago in Dubai.
Another routine victory saw American Madison Keys ease past Jasmine Paolini 6-1 6-1, but there was no such luck for 2020 Australian Open champion Sofia Kenin.
She was dispatched 6-1 6-1 by world number 26 Marie Bouzkova, while Amanda Anisimova claimed a 6-3 6-2 win over veteran two-time grand slam finalist Vera Zvonareva.
Viktoriya Tomova had too much for Kaia Kanepi in a 6-3 6-1 success, with her reward a second-round clash against third seed Jessica Pegula.
World number four Pegula lost to the in-form Iga Swiatek in the Qatar Ladies Open final on Saturday, and Leylah Fernandez will face the Pole next after beating Julia Grabher 6-4 6-2.
Swiatek, who became the first female player to win 25 consecutive matches since Serena Williams in 2015, will face Bianca Andreescu in the last eight after she eased past Petra Martic 6-4 6-4.
"I didn't start well, and everybody could see that," Swiatek told reporters. "I'm really happy with the way I reacted and how I improved in the first set.
"Also how different the second set looked to the first one because I could really reset and really change the way I played. That's the most positive thing for me."
There was a shock in the final game of the day, though, as Daria Kasatkina dumped out number two seed Paula Badosa 6-4 6-4.
Third seed Aryna Sabalenka sealed a third straight win over Jessica Pegula, easing to a 6-1 6-4 victory, while fourth seed Maria Sakkari defeated Coco Gauff 6-4 7-5.
Seventh seed Danielle Collins was knocked out by unseeded compatriot Amanda Anisimova, the 20-year-old cruising past the Australian Open finalist 6-2 6-2.
There were also victories for Jil Teichmann, who overcame Elena Rybakina 6-7 (3-7) 6-3 7-5, and ninth seed Ons Jabeur, who beat Yulia Putintseva 6-3 6-2.
Anisimova came from a set down to beat her compatriot 6-7 (4-7) 6-2 6-1 on Centre Court at Wimbledon.
The American world number 25 has now won 12 matches in three sets in 2022, which is the joint-highest tally on the WTA Tour so far this season, level with Beatriz Haddad Maia.
"It was my first time playing on Centre Court and this is the most special day of my career," the 20-year-old told BBC Sport following her success over this year's French Open runner-up.
"It's just a huge privilege to play on this court playing Coco. She is an amazing player, got to the final of a grand slam, so I wanted to soak up the moment. Winning is so special, especially in front of a full crowd.
"There are so many American players doing well and I'm proud of my country and how we have been doing. It was really exciting to have an all-American clash on this court so it was really special."
Next up for Anisimova in the round of 16 is Harmony Tan, who has been one of the standout stories from the first week at The All England Club.
Tan defeated Serena Williams in the first round, following that triumph up with wins over Sara Sorribes Tormo and Katie Boulter.
The former world number one is enjoying her first SW19 campaign since that triumph three years ago, with the coronavirus pandemic and a calf injury delaying her return.
The final in 2019 was Halep's fifth at a major, but she has not been back to that stage since.
Now, having swatted aside Amanda Anisimova 6-2 6-4 in the last eight for a 12th consecutive victory at Wimbledon – the longest sequence since 20 straight Serena Williams successes between 2015 and 2018 – she is just one win away.
Halep explained after the Anisimova match that confidence was key, having proven her game was back at a high level in reaching six semi-finals in 2022 – second only to Iga Swiatek (eight) on the WTA Tour.
Three of those last-four appearances have now been on grass, with Johanna Konta in 2017 the last player to achieve that feat in a calendar year.
"Definitely I've played the best tennis [since 2019]," Halep said in her on-court interview. "I struggled a lot last year; now, I'm just trying to build my confidence back.
"The tennis is here, so I just have to believe. I've started to do that, and it feels good."
Asked how high her confidence was now, she replied with a smile: "It's good."
Halep has reached the last four without dropping a set, although that spotless record was briefly threatened by Anisimova, who was a double break down in the second set before breaking back and then leading 40-0 on the Romanian's serve.
Yet Halep dug in to serve out the match and avoid a decider against an opponent with a Tour-leading 12 three-set wins this season.
"I'm very emotional right now, because it means a lot to be back in the semis," Halep said.
"I played a tough opponent today; she could crash the ball in the end, and I didn't know actually what to do.
"But I just believed in myself and said that I had to stay there, strong on my legs – they helped me today – and I believed until the end that I could win."
Former world number one Halep took the title at the All England Club in 2019 but had not been back since, with coronavirus wrecking the 2020 grass-court season before she missed its entirety in 2021 due to injury.
But it is as if the 30-year-old – backed by new coach Patrick Mouratoglou – had never been away, with Anisimova the victim of a ruthless display on Wednesday.
Anisimova might have hoped the omens were positive, given her only prior quarter-final win in a major came against Halep at the 2019 French Open, but she could hardly have been surprised by her opponent's dominance on this surface; Halep beat Anisimova in the last eight in Bad Homburg last month.
The American soon bowed to the pressure generated by Halep's return, losing five games in a row after initially holding to love. Halep seized her first two break point opportunities as Anisimova twice aimed tired shots into the net from the back of the court.
A cross-court backhand from Halep fended off Anisimova's first opening, ensuring the Romanian eased through the opener before the second set followed a familiar theme.
Anisimova held comfortably to start but then again found Halep resolute, falling 0-40 down and eventually going a break behind with a wayward forehand. Once more it was a double break when an Anisimova drop shot fell some way short.
Anisimova belatedly forced Halep back as she served for the match, taking the second of two break points and then remarkably claiming a 40-0 lead against the serve next time out.
However, Halep, having briefly lost control, recovered her composure and was able to celebrate when Anisimova blasted wide.
Data slam: Anisimova helpless against Halep on grass
Anisimova has won 12 matches in three sets this season, the joint-most on the WTA Tour, but a fightback always appeared unlikely against her imperious opponent.
After almost three years away from competitive grass-court action, Halep has returned in formidable form. In three tournaments on grass in 2022, she has reached three semi-finals. The last player to make a trio of such appearances in a single calendar year was Johanna Konta in 2017.
WINNERS/UNFORCED ERRORS
Halep – 11/6
Anisimova – 13/28
ACES/DOUBLE FAULTS
Halep – 3/1
Anisimova – 0/1
BREAK POINTS WON
Halep – 4/6
Anisimova – 1/8
