"I'm done," he told The Associated Press at the recent opening of "Transformers: Dark of the Moon" at the Moscow International Film Festival. "I'm sure they will make more of them. It's still a very hot franchise."
The 26-year-old actor has appeared in the last three "Transformers" movies playing kid-next-door Sam Witwicky.
"I love making them (the movies). I love the crew. I love Michael (Bay). I love the cast. I love Sam ... but I don't have anything new to contribute and I don't think there's anywhere to take Sam really," LaBeouf said.
"Transformers 3" earned $37.3 million Wednesday in the U.S. on its first day - a 40 percent drop from its predecessor, "Revenge of the Fallen."
The Transformers trilogy was based on the cartoons of 1980s that were themselves inspired by the Marvel Comics comic book of the same name.
The Associated Press contributed to this report.