I have come to hate hugh jackman as Wolverine. He was good in the first two but ever since then he has become way too different from the comic book character (Atleast the version that I enjoyed reading as a kid, Marvel may be doing some other crap with him currently). The movies have made wolverine a leader and a team player, two things he was not in the comics. Hugh Jackman plays wolverine as too much of a nice guy.
Also, I hate Christian Bale's batman. The movies were great but ironically christian bale as batman was probably the worst thing about those movies.
Robert Downey Jr. is perfect as Tony Stark/Iron Man so he would be my pick.
Andrew Garfield is perfect as spiderman but I don't like his Peter Parker much.
Toby McGuire was decent as Peter Parker but I didn't like his Spiderman.
McAvoy as Professor X should be on the list as well. Visually Patrick Stuart is perfect but I think from an acting stand point McAvoy actually embodied the character better.
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