Yeah I agree with a lot of what's been said... heres some that come to my mind

Kill Bill Vol. 1 & 2 , Bill - So heartless, and calm at all times, David Caradine was great in this role

Hannibal Lecter - Hannibal the cannibal is super creepy, Anthony Hopkin's will kinda creepy in any film cause I always think of Hannibal

Seven, John Doe - He's so self-righteous about it it makes it so much creepier

The Devils Advocate - Al Pacino was great as the devil

Scarface - Gotta mention that one too

Fight Club, Brad Pitt as Tyler Durden

The Warden in Cool Hand Luke

Darth Vader

Denzel's charachter in Training Day, i forget his name