Besides his iconic role as Mr. Spock, Nimoy played Paris on 49 episodes of Mission: Impossible. One of the "cover of the Rolling Stone" moments for TV celebrities back in the show's heyday was playing the guest villain in an episode of Columbo; Nimoy played a surgeon in the episode A Stitch in Crime. The non-Spock I'm most familiar with is his narration in the computer game Civilization IV.
In an uncredited early role, Nimoy played an Army sergeant in Them! The voice doesn't sound like him at all, but that's him. I'm guessing the film director wanted him to speak with a more average-Joe-American accent.
Nimoy's IMDb page is here. His Wikipedia page is here.