The left-hander cracked an unbeaten 149 for his fifth one-day hundred before the West Indies were restricted to 324-8 in reply to India's challenging total of 338-3 on a batting pitch.
India were indebted to Sourav Ganguly for posting their highest total against the West Indies as the left-handed opener celebrated his comeback with a superb 98.
The former Indian captain, playing his first one-dayer in 16 months, hammered three sixes and 11 fours in his 110-ball knock to help the hosts surpass their previous best total of 325-5 against the West Indies.
The 32-year-old Chanderpaul threatened to ruin Ganguly's day with a gem of an innings, which came off 136 balls with the help of three sixes and 16 fours. He was named man of the match.
The West Indies matched India in the early stages when they raced to 80 in 12 overs, thanks to Chris Gayle who punished the pacemen with a wide range of shots to hit 10 fours in his 46-ball 52.
The run-rate declined after the dismissal of Gayle, caught in the slips by India skipper Rahul Dravid off spinner Harbhajan Singh. The spinner struck again when he bowled Runako Morton to reduce the West Indies to 102-2.
Chanderpaul sustained the West Indies' hopes, but the asking-rate kept climbing as they needed an exact 100 to win in the closing 10 overs with seven wickets in hand.
Skipper Brian Lara scored a brisk 31 before falling in a bid to step up the run-rate. India then looked in control despite Chanderpaul's heroics.
India's batting flourished in the morning session, much to the delight of a sizeable Sunday crowd. Ganguly and Gautam Gambhir (69) put their team on course for a big total with a 144-run stand for the opening wicket.
Wicketkeeper-batsman Dhoni (62 not out) and Dravid (54 not out) built on the openers' efforts, exploding with a flurry of boundaries to add 119 vital runs for the unfinished fourth wicket in the closing 11.5 overs.
Lara's decision to put India in to bat after winning the toss failed to produce instant results as his team had to wait for nearly 25 overs for the first success.
Off-spinner Gayle provided the breakthrough when he had Gambhir caught cutting by Marlon Samuels. Gambhir, playing his first one-dayer after nine months, hit 10 fours in his second half-century.
But there was no stopping Ganguly, who batted with authority against both seamers and spinners. His aggressive knock helped India maintain an impressive run-rate from the beginning.
Ganguly put on 70 for the second wicket with Sachin Tendulkar, a specialist opener batting at the number-three position. Tendulkar contributed 31 before being trapped leg-before by Gayle.
Ganguly looked set to complete his 23rd one-day century when he was run out following a superb piece of fielding by Dwayne Smith, who picked the ball cleanly and hit the stumps at the non-striker's end.
Runs continued to flow after Ganguly's dismissal as Dhoni and Dravid dominated the attack in the closing overs.