The Warden in Holes, although I think she was nastier in the book.
Definitely a little off topic, as he’s certainly not one of the top 5 villains, but I truly enjoyed Gary Oldman as Egor Korshunov in Air Force One. This isn’t his highest-rated role (that would be his role in Tinker, Tailor, Soldier, Spy), but he’s one of my favorite actors and he takes this villainous role and makes it sing.
Frank Langella as the White House chief of staff in Dave
Magua from The Last of the Mohicans
Darth Vader from the Star Wars movies
Maj. Strasser from Casablanca
Dolores Umbridge from the Harry Potter movies
Come on, boys and girls 2 pages and still no Richard Boone for Hombre?
Dr. Evil (Austin Powers) 
He’s not the villain though, Angel Eyes is. Tuco’s the closest thing the flick has to a hero (Blondie being a complete jerk)
I’ll second Hans Landa. That character was so *cheerfully *terrifying. That first scene, where he politely interrogates the farmer, knowing *exactly *what’s up but delighting in the poor guy’s terror was simply chilling.
Honorable mention for Jeremy Irons as Damodar in Dungeons & Dragons. A shit role in a truly abysmal movie, saddled with exclusively eye-roll worthy lines… and he just delights in chewing the scenery regardless. You can really tell he’s having a ball playing the Evilest Lord of Evil that Ever Eviled.
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The doctor from “The Human Centipede”
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The raping Hillbillies from “Deliverance”
Good one. Although…BR is a film I never get tired of watching, and there are times when I think Roy is in fact the “Tragic Hero” of BR. More human than human, and ultimately more humane than human.
He was also great as the Über-Morlock in the 2002 version of The Time Machine. Scared the crap out of me! :eek:
According to Wiki, Cusack never played George Smiley:
Ooo, good one. Similarly, but not exactly, Ozymandias in Watchmen.
You are right: he played Control.