The left-hander smashed 13 fours and three sixes before retiring to the pavilion as the West Indies piled up 344-5 from 45 overs against a Gujarat team at the Motera stadium here on Wednesday.
Runako Morton hit a run-a-ball 91 during a second-wicket stand of 227 with Gayle and Wavell Hinds made 61 off 58 balls.
The tourists won by 173 runs as the locals were restricted to 171-6 despite batting for 50 overs. Seamers Corey Collymore, Dwayne Smith and Dwayne Bravo picked up two wickets each.
The West Indies, who won the previous Champions Trophy tournament in England in 2004, open their campaign with a qualifying match against Zimbabwe on Sunday.
Brian Lara's men will also play Sri Lanka and Zimbabwe in the round-robin league with the top two advancing to the main tournament against Australia, South Africa, India, Pakistan, New Zealand and England.
West Indies 344 for 5 in 45 overs (C. Gayle 101 retired, R. Morton 91, W. Hinds 61, A. Makda 3-65)
Gujarat XI 171 for 6 in 50 overs (N. Patel 37, C. Collymore 2-45, D. Smith 2-16, D. Bravo 2-21)