Deebo, but he makes a good meathead bad-boy to Bow Wow's "lucky" scapegoat. But Sweet Tee's the guy that gave me chills - a too-slick fat-cat who keeps the projects under his thumb.
Cyrus - "Cyrus" - Not so much a villain as an Oedipal cock-block, Cyrus is a major drag.
Lieutenant Terence McDonagh - "The Bad Lieutenant: Port of Call - New Orleans" - He's too redemptive to be a villain but Nic Cage's madcap performance is awesome. Also in the much-maligned category.
Red Mist - "Kick-Ass" - The Red Mist's turn was tragic. Hopefully he lives up to his closing words in the upcoming "Kick-Ass 2."
Might have made this list if I had gotten around to seeing the films (it's been a busy semester):
Dr. Heiter - "The Human Centipede"
Bronson - "Bronson"
If I missed any, lemme know!