I like Jeff Bridges a lot. I think he's best in drama movies where he plays vulnerable characters, like The Fisher King or Crazy Heart, even if he's mostly remembered as the guy who played The Dude (The Big Lebowski).
Bill Murray's characters may not always be that diverse, but they are always interesting to watch. Back in the day, he was funny and sarcastic (Groundhog Day, Ghostbusters) while later in his career, his roles tend to be more introverted, quirky and fun to watch. Especially in Wes Anderson films like Rushmore or The Life Aquatic with Steve Zissou!
I've a few times been impressed with Christian Bale and how dedicated he is as an actor, for example how he starved himself for his part in The Machinist.
He's one of those actors that can seem like an entirely different person depending on the movie. Still, his characters always seem "off" in some way and he's not yet played a dramatic role in which I really sympathized with him. I would love to see him pull that off, though.
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Originally Posted by eric generic
honorable mention but he doesn't do enough films: Jack Nicholson (The Departed).
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There are many good movies if you go back in time, f.ex One Flew Over the Cuckoo's Nest, Chinatown or The Shining.