I have problems with this because there are so many small nuances to a performance. I might love one for the comedic factor, but then another for the drama. They don't really lend themselves to listing out in my skull. : /
But here's a few I thoroughly enjoyed.
Robin Williams in Patch Adams
Tim Robbins in The Shawshank Redemption
Chris Tucker in The 5th Element (Because it is damned hard to play a metrosexual diva in the 25th century...)
Sigourney Weaver in Gorillas in the Mist
Michael Clark Duncan in The Green Mile (I loved the books and the movie makes me cry ever...single...time.)
And...sadly...I can't really come up with too much else. I'm going to blame that on the fact I just woke up. Heh. :D
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