Mark Ruffalo as Bruce Banner (The Avengers)
Tom Hardy as Bane (The Dark Knight Rises)
Gary Oldman as Commissioner Gordon (The Dark Knight trilogy)
Stephen Rea as Eric Finch (V for Vendetta) (I just love Stephen Rea, okay)
Billy Crudup as Dr. Manhattan (Watchmen)
Clive Owen as Dwight McCarthy (Sin City)
Benecio Del Toro as Jackie Boy (Sin City)
Willem Dafoe as Norman Osborn (Spider-Man)
Jeffrey Dean Morgan as The Comedian (Watchmen)
Heath Ledger as The Joker (The Dark Knight)
Hugo Weaving as V (V for Vendetta)

And I'll second Mickey Rourke as Marv for Sin City. He was so, so perfect. I haven't seen The Wrestler and I've heard that was his best performance, but man, him as Marv was great.

I think Toby McGuire played a good dweeby little geeky Peter Parker, which was kindof how I always imagined him. I don't particularly like Toby McGuire, though, and I don't think he particularly played his Spidey parts well. And also the movies weren't that great.

I'm sick to death of Iron Man. Sue me.