Bolt, who owns the 100-meter world record at 9.58 seconds and the world 200m record of 19.19, spoke Friday on the eve of his opening race of the 2016 campaign in the Cayman Invitational.
The Jamaican superstar has long been critical of Van Gaal's stewardship of Manchester United, saying he has not used players in the proper positions and that has led to disappointing performances by the English Premier League club.
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"I supported Manchester United for years," Bolt said. "I would still love to play for them, but if Louis Van Gaal is the coach, not so much," Bolt said.
Manchester United stands fifth in the Premier League with 18 wins and 9 drawn from 37 starts entering Sunday's season-ending matches, two points behind fourth-place Manchester City.
Bolt, who predicted he will open his season by running the 100 in 9.91, will face only two sub-10 sprinters at the Truman Bodden Sports Complex -- Jamaica's Kemar Bailey-Cole and Kemar Hyman of Cayman Islands.
Last week, Bolt told TV2 Norway of his thoughts about Manchester United's season.
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"It has been up and down. I wouldn't say I'm happy. I think a lot of players don't want to come to the team under Van Gaal. I think players don't want to play for him," Bolt said.
"He plays a different style of football which Manchester United doesn't really play. We are more of an attacking team and he likes to pass the ball. I'm not saying he's not a good coach but, personally, I just think he's not right for Manchester United."
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