Rahul was supposed to feature in India's tour of West Indies last month after recovering from a hernia operation, but missed out after testing positive for COVID-19.
The 30-year-old will now return to lead his country for the second time in the 50-over format after receiving medical clearance to play, with Shikhar Dhawan vice-captain.
India fell to a 3-0 series defeat in South Africa when Rahul last captained the team this year, and the batter has not played any competitive cricket since the conclusion of the 2022 Indian Premier League season.
Rahul hit an ODI century on his debut against Zimbabwe back in 2016, the first of five hundreds in the format.
The three-match series gets under way at Harare Sports Club on August 18.
India squad: KL Rahul (captain), Shikhar Dhawan, Ruturaj Gaikwad, Shubman Gill, Deepak Hooda, Rahul Tripathi, Ishan Kishan, Sanju Samson, Washington Sundar, Shardul Thakur, Kuldeep Yadav, Axar Patel, Avesh Khan, Prasidh Krishna, Mohammed Siraj, Deepak Chahar.
Half-centuries from Shikhar Dhawan and skipper Shreyas Iyer accounted for the bulk of the Capitals' 161-7.
Ben Stokes (41) and Jos Buttler (22) impressed at the top of the Rajasthan reply but neither man could kick on and when Anrich Nortje (2-33) crowned a blistering fast-bowling display by bowling Robin Uthappa for 32, the task was beyond a Royals side who have now lost five of their eight games in the competition.
Jofra Archer gave Rajasthan the perfect start with a beautiful delivery that nipped back off the seam to bowl Prithvi Shaw from the first ball of the match.
That launched a stunning opening burst of 2-5 from the England paceman, who Ajinkya Rahane pulled tamely to mid-on.
Dhawan played with typical authority until his 33-ball stay ended in inauspicious fashion on 57 when he scooped Shreyas Gopal to Kartik Tyagi at third man.
Iyer passed fifty when a third umpire review showed Stokes had the ball in his hand and a foot grounded behind the rope when attempting to take a catch off Jaydev Unadkat.
The Capitals captain holed out for 53 off Tyagi next over and the end of their innings brought a clatter of wickets, with Archer (3-19) and Unadkat (2-32) the beneficiaries.
Stokes clipped the opening ball of the Royals' reply for four and he and England team-mate Jos Buttler ensured an explosive initial response.
South Africa paceman Nortje elected to meet fire with fire and, having been thumped over wide long-on for six and scooped for a pair of fours, he bowled Buttler to end an undulating nine-ball stay.
Rajasthan's promising start went further off the rails when Smith continued poor recent form by chipping a return catch to Ravichandran Ashwin for one.
Stokes looked in immaculate touch and hit six fours in his 41 before misjudging Tushar Deshpande's slower ball to be caught in the deep by substitute Lalit Yadav.
Sanju Samson hit Axar Patel over midwicket for a monstrous six that resulted in the retrieved ball being changed but the left-arm spinner had his revenge, bowling the big-hitter for 25.
Patel then accounted for Riyan Parag via a run out - a debacle for which Uthappa was unable to atone as his team-mates limped to148-8.
Pace like fire
The pitches of Dubai are rarely thought of as the ideal stage for the world's premier fast bowlers but Archer and Nortje put on a thrilling exhibition of their art. Of the five runs Archer conceded in his opening spell, only two came off the bat.
If none of the Delhi Capitals line-up could get the measure of Archer, the same could not be said about the Royals' batsmen's ability to deal with Nortje initially, as Buttler threatened to dispatch him to all parts.
The solution? Bowl faster. And faster still. The delivery that bowled Buttler and the one he ramped preceding it both touched 156 km/h. It was a gripping battle.
Smith gets it wrong
Normally so reliable with the bat, Smith's form has fallen away dramatically. This was his fifth single-figure score in six innings and the Australia star also fell short with his captaincy.
The decision to remove a rampant Archer from the attack after two overs looked questionable at the time and it felt like Delhi had been decisively let off the hook as Dhawan and Iyer compiled their crucial 85-run stand.
Shaw hit 11 fours – including six in a row in one over – and a trio of sixes in an innings of 82 that helped the Capitals coast to a 155-run target at the Narendra Modi Stadium in Ahmedabad.
Shikhar Dhawan was happy enough to play second fiddle to his opening partner, making 46 from 47 balls before falling lbw to Pat Cummins with the total on 132 in the 14th over.
Cummins (3-24) also removed the outstanding Shaw and Rishabh Pant (16) with the finishing line in sight, leaving Marcus Stoinis to complete the job with a streaky four as Delhi triumphed with 21 balls to spare.
Kolkata had been indebted to some big hitting in the closing stages from Andre Russell but still finished with a below-par 154-6. The all-rounder blasted two fours and four sixes to top score with 45 not out.
Their hopes of posting a more substantial total had been damaged by losing four wickets for 13 runs in the middle overs, seeing them slip from 69-1 to 82-5.
Shubman Gill made 43 at the top of the order but both captain Eoin Morgan and Sunil Narine failed to trouble the scorers amid the collapse.
Lalit Yadav finished with figures of 2-13 for Delhi, while Axar Patel (2-32) also struck twice with his left-arm spin to help restrict the Knight Riders, who have now lost five of the past six meetings between the teams.
Double celebration for Russell
Russell celebrated his 33rd birthday with an eye-catching 27-ball knock that saw him surpass 6,000 Twenty20 runs in his career.
The right-hander was cautious at first before cutting loose, smashing Kagiso Rabada for successive sixes to finish the 19th over before ending the 20th with another off the bowling of Avesh Khan.
Capitals gain from a Shaw thing
Shaw reached his half-century from just 18 deliveries, aided by taking Shivam Mavi for six successive fours in an opening over that cost 25 runs (Delhi's reply had started with a wide).
Delhi's fifth victory in seven outings in the 2021 season sees them move level on 10 points with leaders Chennai Super Kings and Royal Challengers Bangalore in the table.
Smith struck a sensational 105 from just 66 balls and Finch crafted 114 in Australia's massive total of 374-6 - their biggest against India in the 50-over format.
David Warner (69) also made the tourists suffer, while Glenn Maxwell bludgeoned 45 from only 19 balls in Australia's second-highest ODI total at the SCG.
Mohammed Shami (3-59) was comfortably the pick of the India bowlers on a painful Friday afternoon in the field.
Hardik Pandya struck a superb 90 and Shikhar Dhawan made 74, but India, returning to action for the first time since March due to the coronavirus pandemic, fell short on 308-8 in reply.
Josh Hazlewood (3-55) and Adam Zampa (4-54) did the damage with the ball for Australia as they started their summer in style to go 1-0 up in the three-match series.
FINCH AND WARNER MAKE HISTORY
Finch and Warner combined for the highest opening stand for Australia in an ODI at the SCG, their 156 surpassing the record of 152 set by Geoff Marsh and David Boon in 1986.
Shami finally got the breakthrough in the 28th over, snaring Warner caught behind after Virat Kohli reviewed, but Finch and Smith dished out more punishment, putting on 108 in just 12 overs.
The brilliant Finch struck two sixes and another nine fours in his fourth ODI century against India, a tally only Ricky Ponting has bettered with six, before the skipper became Jasprit Bumrah's only victim.
SENSATIONAL SMITH AND MAXWELL GO BESERK
While Finch uncharacteristically scored at less than a run a ball, Smith raced to a magnificent hundred which he reached off 62 balls.
Smith failed to hit the heights during the recent Indian Premier League but produced a disdainful knock as he dispatched the tourists' attack to all parts - Yuzvendra Chahal (1-89) conceding the most runs by an India spinner in an ODI.
The imperious Smith hit four sixes and 11 fours as he put on a show along with Maxwell, who treated the crowd to some astonishing innovative strokes in an explosive innings.
HAZLEWOOD AND ZAMPA DERAIL INDIA CHASE
India's run chase got off to a blistering start, Mitchell Starc conceding 20 off an 11-ball first over, but they were struggling on 101-4 in the 14th over - Kohli making just 21 after he was dropped by Zampa on one.
Hazlewood had Kohli caught by Finch at midwicket and the quick also saw the back of Mayank Agarwal and Shreyas Iyer.
Dhawan - dropped by Maxwell on 41 - and Pandya - playing as a specialist batsman - gave India hope with a fifth-wicket stand of 128, but spinner Zampa removed both in quick succession and got rid of Ravindra Jadeja in an ultimately comfortable win for Australia.
The start of the series was delayed by five days due to a coronavirus outbreak in the Sri Lanka camp, with batting coach Grant Flower and team data analyst GT Niroshan testing positive for the Delta variant.
Sri Lanka's squad were allowed to leave isolation and resume their preparations last weekend after returning negative PCR tests.
ESPNcricinfo reported team doctors believed Flower and Niroshan's infections stemmed from the recent tour of England, where the home team suffered a breach of their bio-secure bubble that forced them to name a reserve line-up for their subsequent ODI games against Pakistan.
Although Sri Lanka do not find themselves in quite such a selection bind, they remain without deposed captain Kusal Perera due to a shoulder injury and Niroshan Dickwella, Kusal Mendis and Danushka Gunathilaka remain suspended for breaking COVID-19 protocols during the England tour.
Dasun Shanaka will skipper the team, a previously bit-part white ball player having ascended to the role amid a stand-off between Sri Lanka's players and their board over playing contracts.
They will emerge from a troubled period to take on an India side captained by opener Shikhar Dhawan and with pace bowler Bhuvneshwar Kumar second in command.
India batting great Rahul Dravid has been named as coach for the tour, with the first-choice side awaiting their forthcoming series in England.
Batsmen Devdutt Padikkal, Ruturaj Gaikwad and Nitish Rana, all-rounder K Gowtham and left-arm seamer Chetan Sakariya have all been handed maiden call-ups.
Bhuvi ready to put injury woes to one side
Kumar will be the leader of fast bowling unit also featuring Sakariya, Navdeep Saini and Deepak Chahar. Having been beset by injury problems over recent years, he was back to his best in the March limited-overs series against England. In the ODIs, he took six wickets at a miserly economy rate of 4.65.
Shanaka must show leadership class
Irrespective of how and why Shanaka became Sri Lanka captain, he is now the man in possession of a role that tends not to promise longevity for incumbents. He will need to improve upon 611 runs and 10 wickets from his 28 ODI appearances to date to turn some unhelpful conversations around.
Key Opta facts
- India are undefeated in their past 11 ODI series against Sri Lanka (W9, D2). Their previous defeat was a 3-0 reverse way back in 1997.
- India have won each of eight most recent ODIs in Sri Lanka, all versus the host country. It is a streak that began after a nine-wicket loss in 2012.
- Sri Lanka have at least won their past five ODIs at the R. Premadasa Stadium. The last time they enjoyed a longer winning run at the venue in this format was a six-match span from December 2001 to September 2002.
- Dhawan will become the 25th player to captain India in ODIs. He requires 23 more runs to become the 10th Indian player to register 6,000 runs in 50-over internationals.
Man-of-the-match Shikhar Dhawan laid a solid foundation for India with an assured 98, missing out on three figures when he miscued a pull off Ben Stokes to Eoin Morgan at midwicket.
Kohli made a similarly fluent half-century but the hosts had stumbled to 202-5 when debutant Krunal Pandya joined KL Rahul in the 41st over.
Krunal (58 not out) laid waste to an otherwise impressive England bowling performance, his 26-ball fifty the fastest ever in a maiden ODI, while wicketkeeper Rahul similarly impressed with an unbeaten 62 as India posted 317-5.
England threatened to make short work of that total as Jonny Bairstow (94) and Jason Roy (46) motored to 135 without loss inside 15 overs, before India's seamers turned the contest on its head.
Prasidh Krishna, also on debut, was the pick with 4-54, while Shardul Thakur's 3-37 accounted for the dangerous trio of Bairstow, Morgan (22) and Jos Buttler (2), and the excellent Bhuvneshwar Kumar took 2-30.
"That's one of our sweetest victories in the recent past. We haven't won many good games in ODIs," India skipper Kohli said at the post-match presentation.
"It was a great comeback from all our bowlers after going for few runs early on. Prasidh was amazing, Krunal as well. Shardul, Bhuvi were amazing. I am a really proud man right now.
"The team showed great character and intensity. As I've mentioned in the past as well, we promote players who have intent and back their skills.
"A special mention to Shikhar's innings as well and KL was back among the runs. We want to back people who will do a selfless job.
"It's a healthy competition between everyone for every slot. We have two or three players available for every slot."
Perhaps not to quite the same extent, but world champions England have their own enviable depth of talent.
Nevertheless, the steadying hand of Joe Root at number three, where Stokes stepped up to be dismissed for one, and Jofra Archer's death bowling were certainly missed as both players undertake a period of rest.
As in the recent 3-2 reverse in the T20I series, captain Morgan was left to rue middle-order failings, with the plummet form 135-0 to 176-5 key in England's challenge fading to 251 all out with 47 deliveries unused.
Nevertheless, he stood by the aggressive approach that has brought his side so much recent success.
"I thought the bowlers were outstanding and there was a bit more on offer for their seamers," he said.
"The two openers were outstanding, but we failed to build on from that. We need to execute better than we did. India did really well and deserved to win.
"Being able to take the attack to the opposition is something that we pride ourselves on. We want to continue to push the envelope in that regard. It's better for us to lose like this than losing by 20 runs.
"The game is always moving forward, technology and fitness are moving forward, so we need to push hard as we can. It's important for us to dictate the way we play."
Punjab captain Dhawan, who was dropped twice by Bhuvneshwar Kumar, fell agonisingly short of three figures against his former side, blasting the last ball for six to drag the Kings to 143-9 in Hyderabad.
Mayank Markande had rattled through the Punjab batting line-up with an incredible 4-15 through the middle overs before Dhawan contributed to 52 of the 55-run last-wicket stand with Mohit Rathee (1 not out).
Sam Curran (22) was the only other Kings batter to hit double figures as Marco Jansen (2-16) and Umran Malik (2-32) impressed, although the Sunrisers allowed Punjab back into the game after they were 88-9.
Hyderabad made a stuttering start to their chase as Harry Brook fell for 13 when bowled by Arshdeep Singh (1-20) before Rahul Chahar (1-28) removed Mayank Agarwal (21) to leave the hosts 45-2 after 8.3 overs.
But Tripathi stepped up with an expert 74 from 48 deliveries, combining with Sunrisers skipper Aiden Markram (37 not out) in a vital 100-run partnership to see Hyderabad over the line with 17 balls left.
Bhuvneshwar sets early tone for Sunrisers
Bhuvneshwar (1-33) dismissed Prabhsimran Singh leg before wicket with the first ball of the match to set the tone, albeit his erroneous catching efforts afforded Dhawan two lifelines later in the Kings innings.
Veteran star Bhuvneshwar has dismissed an opening batter 55 times in the IPL, the most by any seamer in history and third among all bowlers (Ravichandran Ashwin and Harbhajan Singh have 61 each).
Non-existent support for remarkable Dhawan
Dhawan was left without support despite his incredible effort. He accounted for 69.2 per cent of his side's total, the second-highest percentage of a team's runs in IPL history when batting first (after Brendon McCullum scored 158 not out in Kolkata Knight Riders' 223 versus Royal Challengers Bangalore in 2008).
Opener Dhawan smashed 12 fours and cleared the ropes five times in his well-crafted 66-ball innings, becoming the leading run scorer in the embryonic IPL batting charts after taking his tally to 225.
Aaron Finch and David Warner dominated proceedings as Australia cruised to a 10-wicket victory with 12.2 overs to spare in response to India's disappointing 255 all out at Wankhede Stadium on Tuesday.
A miserable start to the three-match series saw India captain Kohli caught and bowled by Adam Zampa for 16 just after he had hit the spinner for six.
Kohli is the world's number one batsman in the 50-over format but 16 is in fact his highest score from fourth in the order as part of a dreadful seven-innings streak that dates back to January 2015.
"We've had this discussion many times in the past," Kohli, who dropped down the order after Rohit Sharma's return, said to Star Sports.
"Because of the way KL Rahul has been batting, we have tried to fit him in the batting line-up.
"Having said that, I don't think it's quite gone our way whenever I've batted number four, so we'll probably have to rethink about that one.
"All in all, it's about giving some guys opportunities and you'll never know if this works or not if you don't try.
"It's very easy to just go with one template and just follow it non-stop. I think people need to relax and not panic with one game, I'm allowed to experiment a little bit and fail as well at times.
"You lose games here and there, but this was one of the days where it didn't come off."
Rahul (47) put on 121 for the second wicket along with Shikhar Dhawan (74), but his dismissal proved the turning point for Australia's bowlers, as India quickly fell to 164-5.
Set 256 to win, Warner (128 not out off 112 balls) and Finch (110no from 114) enjoyed a day to remember with the highest opening stand in an ODI against India, leaving the hosts with plenty to think about before the second game in Rajkot on Friday.
"It's just one bad day at office," added Dhawan. "We played well against West Indies before. As a team we back each other, and we don't focus too much on a loss.
"They played really well. We were a bit unlucky as well, like a few top edges went here and there, they didn't go in the hand.
"When KL got out, at that time we planned to accelerate and those four wickets we lost, that's where we lost the momentum.
"From there, we were targeting 300 runs and because of loss of wickets we ended up scoring less runs on that sort of a wicket. In bowling, we could not take wickets and they outplayed us. It is the captain's choice [where he bats]."