At least according to the "Time" magazine of May 7, 2007.
Arranged by the year, the film was released.
1945 "Detour" Vera (Ann Savage)
1949 "White Heat" Cody Jarrett (James Cagney)
1962 "Cape Fear" Max Cady (Robert Mitchum)
1962 "The Manchurian Candidate" Mrs. Iselin (Angela Lansbury)
1972 "Aquirre, the Wrath of God" Don Lope de Aguirre (Klaus Kinski)
1976 "Marathon Man" Dr. Christian Szell (Laurence Olivier)
1984 "The Terminator" The Terminator (Arnold Schwarzenegger)
1993 "Schindler's List" Amon Goeth (Ralph Fiennes)
1994 "Pulp Fiction" Marsellus Wallace (Ving Rhames)
2001 "Hannibal" Hannibal Lecter (Anthony Hopkins)
Any additions? Deletions? Comments?
I'll hold most of my comments to later on, but I do have two quick comments now. Note that most of these actors and actresses were born somewhere else other than the U.S. And that most of these villains are fairly well known, except for perhaps the first one.
Many good ones there, people. Here are mine. First, in alphabetical order, a score of greats, who made the greatest (IMHO) villains. Notice that most of them were born somewhere other than the U.S., which goes to my supposition that dem dere foreigners make better villains than we Americans.
Lionel Atwill
Humphrey Bogart
James Cagney
John Carradine
Lon Chaney, jr.
Hans Conreid
Peter Cushing
Henry Daniell
Gert Froebe
Lionel Jeffries
Boris Karloff
Christopher Lee
Peter Lorre
Bela Lugosi
Vincent Price
Basil Rathbone
Edward G. Robinson
George Sanders
Terry-Thomas
George Zucco
And some one-shot villains. Not necessarily these, but the problem I have with the list from "Time" magazine, is that so many are well known. If you take some of the more obscure villains, I think you'll find them as good or as better than the ones on "Time's" list.
1964 "The Gorgon" Carla Hoffman (Barbara Shelley)
She turns men's hearts to stone, and all the rest of them as well.
1964 "Masque of the Red Death" Juliana (Hazel Court)
Any woman that deliberately brands herself has issues.
1966 "The Reptile" Anna Franklyn (Jacqueline Pierce)
She has a wicked love bite.
1968 "Oliver" Bill Sikes (Oliver Reed)
1968 "2001: Space Odyssey" HAL (Douglas Rains)
"I don't think I can do that."
1971 "Countess Dracula" Countess Elisabeth (Ingrid Pitt)
1971 "Macbeth" Lady Macbeth (Francesca Annis
I can see her telling her husband, if you don't kill the old king and make me the new queen, you'll be sleeping on the couch tonight and every night thereafter.
1971 "Straw Dogs" Tom Hedden (Peter Vaughan)
1988 "Lair of the White Worm" Lady Sylvia Marsh (Amanda Donohoe)
She has a wicked love bite, too.
And a group I'll count as one.
1972 "Tales from the Crypt" Jeanne Clayton (Joan Collins), Ian Hendry (Carl Maitland), James Elliott (Robin Phillips), Ralph Jason (Richard Greene), and Major William Rogers (Nigel Patrick)