Hoffman was the first I thought of when I saw the thread title. He's been fantastic in everything I've seen him in. Two small budget films he starred in recently, Owning Mahoney and Love Liza, were as good as they were strictly because of him. I agree with William H. Macy and John C. Reilly too.
Some other favorites who are somewhat unappreciated:
Paul Giamatti
John Turturro
David Morse
J.T. Walsh (who, unfortunately, died a few years ago)
Steve Buscemi
Clancy Brown
Chris Cooper
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Persuaded, paraded, inebriated, and down
Still aware of everything life carries on without
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