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My favorites...
1) Nurse Ratched (Louise Fletcher), One Flew Over the Cuckoo's Nest
2) Frank (Henry Fonda), Once Upon A Time in the West
3) Noah Cross (John Huston), Chinatown
4) Mrs. Iselin (Angela Lansbury), The Manchurain Candidate
5) Norman Bates (Anthony Perkins), Psycho
6) Hans Gruber (Alan Rickman), Die Hard
7) Harry Lime (Orson Welles), The Third Man
8) Reverend Harry Powell (Robert Mitchum), Night of the Hunter
9) Kasper Gutman (Sydney Greenstreet), The Maltese Falcon
10) Minnie Castavet (Ruth Gordon), Rosemary's Baby
*special mention: the HAL-9000 (voiced by Douglas Rain), 2001: A Space Odyssey
and favorite comic villains...
1) Dean Vernon Wormer (John Vernon), Animal House
2) Dr. Einstein (Peter Lorre), Arsenic & Old Lace
3) Prince Humperdink (Chris Sarandon), The Princess Bride
4) Leonard Smalls - the Lone Biker of the Apocalypse (Randall "Tex" Cobb), Raising Arizona
5) Hedley Lamarr (Harvey Korman), Blazing Saddles
6) Lex Luthor (Gene Hackman), Superman: the Movie
7) Beetlegeuse (Michael Keaton), Beetlejuice
8) Doctor Evil (Mike Meyers), Austin Powers: International Man of Mystery/the Spy Who Shagged Me
9) Mr. Franklin Hart Jr. (Dabney Coleman), 9 to 5
10. Ray "Bones" Barboni (Dennis Farina), Get Shorty
And on and on and on....