I'd go with DannyMontana with Robert De Niro as Al Capone in The Untouchables because I don't really consider Joe Pesci's character in Goodfellas to be a villain persay. I see him not as a good guy, but not as the villain either. Make any sense? Like villian to me either Capone or The Turk in Godfather, Sosa in Scarface, etc.