The Adventures of Tintin star told his followers on Twitter that current Who star Matt Smith is the best man for the role.
"Why is everyone speculating about who should play the Doctor in the Doctor Who movie?" he asked. "Matt Smith is the Doctor, he should f**king play him!!"
Pegg added that he has no interest in returning to Doctor Who following his guest stint in 2005 episode 'The Long Game'.
"It's nice to be thought of but I do not want the part [of the Doctor] and would not accept if it were offered to me," he wrote. "I did my Who time and I died. The end."
Matt Smith confirmed last year that he would be eager to star in a Doctor Who film.
"I would be thrilled if there could be a movie version," he said. "I want them to do it. There is something brilliantly televisual about Doctor Who but I think it could definitely work as a film."
A short Doctor Who sketch will also air as part of this year's Children In Need broadcast on Friday, November 18.
The sci-fi drama will return to BBC One this Christmas for a festive special.
> Doctor Who movie: Does it work on the big screen?
Watch Simon Pegg filming on Doctor Who below: