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Joaquin Phoenix in Gladiator

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You can't be serious.

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That character affects me when I watch that movie more than just about any other I can think of. You could hook me up to a heart monitor and watch it go though the roof anytime he's on screen.

It drives me crazy because I really can't enjoy the movie as much as I could if someone else played that character, but I do think it's because he was so good in the roll.

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George Clooney - O'Brother Where Art Thou

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ooooh, yes, forgot about that one! good pick

Already posted:
Brad Pitt - 12 Monkeys
Denzel Washington - Malcolm X
Johnny Depp - Pirates of the Caribbean: The Curse of the Black Pearl
Leonardo DiCaprio - The Aviator
Val Kilmer - Tombstone
George C. Scott - Patton

Not yet posted (or I overlooked):
Daniel Day Lewis - In the Name of the Father
Kevin Bacon - Murder in the First
Forest Whitaker - The Last King of Scotland
Robert Downey Jr. - Tropic Thunder
Paul Newman - The Verdict

I'm changing my answer.

Bill Paxton in Aliens.

Two that absolutely transformed into the role:

Sissy Spacek in Coal Miners Daughter
Neil Patrick Harris in Harold & Kumar

Didn't see my personal favorite mentioned - Eli Wallach as Tuco.

Van Kilmer Doc Holiday

Billy Bob Thorton - Sling Blade

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Paris Hilton - House of Wax.

EOT.

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