Nimoy made a splendid adversary to LAPD detective Columbo in the 1973 episode 'A Stitch In Time'[1]. I'm surprised that the New York Times article doesn't mention it at all because it is one of the best Columbo episodes, with a couldn't-see-it-coming twist in the end.

[1] http://www.imdb.com/title/tt0069900/

Incidentally, William Shatner played the villain in 2 episodes of Colombo: 'Fade in to Murder' (1976) [2] and 'Butterfly in Shades of Grey' (1994) [3].

[2] http://www.imdb.com/title/tt0074328/

[3] http://www.imdb.com/title/tt0109458/

Apple fanbois will be interested to learn that Columbo loved to use the innocent-sounding phrase "Just one more thing ...." while faking an exit.

I really liked him in the 1978 'Invasion of the Body Snatchers' : http://www.imdb.com/title/tt0077745/

Fringe. He doesn't appear until well into the show, but he definitely steals the spotlight.

I was amazed to recently have found out that he played the voice of Galvatron in the original Transformers movie (which was amazingly not-sucky compared to the series).

He has a long list of roles as a voice actor.

His books are probably a good way to start.