Five off the top of my head (In no order):

Bob Gunton as Warden Norton - The Shawshank Redemption


Lee J. Cobb as Juror #3 - 12 Angry Men


Robert Patrick as the T-1000 - Terminator 2: Judgment Day


Leandro Firmino as Zé Pequeno/Li'l Zé - City of God


Robert De Niro as Neil McCauley - Heat