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The 35-year-old West Indies left-hander, renowned as one of the most dynamic batsmen in world cricket today, struck 10 fours and 15 sixes as he made a stunning 151 not out off just 62 balls at Taunton's County Ground.
Yet Kent still came away with a three-run win after they defended a total of 227 for seven that featured Sam Northeast's 114.
Gayle could only watch as Somerset slumped to 22 for two before the powerful Jamaican smashed three sixes in eight balls.
The big hits kept coming, three balls disappearing out of the ground landing in the nearby River Tone.
But Australian seamer Mitchell Claydon starred with the ball, the seamer doing well at both ends of the innings on his way to two for 23 in his maximum four overs.
Somerset coach Matthew Maynard, an aggressive batsman in his playing days, said: "I thought Sam Northeast played a sensational innings, but then the world boss came in and it's different gravy.
"Words can't explain exactly what we have seen today. He makes it looks so easy and strikes the ball so cleanly. His knock almost brought off an incredible win today, but it just wasn't to be," former England international Maynard added.
Gayle kept Somerset in sight of victory until the penultimate ball and disbelieving Kent skipper Northeast said: "I don't know where to start.
"It was an incredible game and Chris's innings was one of the best things I have ever seen.
"But special credit has to go to our bowlers, who stuck to their plan and kept believing.
"We were trying to get the other batters on strike, but you miss your length against him and it goes out of the park."
He added: "When the opposition needs 15 an over, you kind of think it's game over.
"But when Chris is out there and it went up to 20 needed off each over, you still know that he can do it. He is an incredible player."
