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You two have already hit many of the big ones. Mine aren't all household names, by any means (although you can easily pick out which ones are, obviously.)
Films:
Agent Smith
Keyser Soze
Clarence Boddicker
Angel Eyes
Monsters:
Godzilla
Audrey II
The Thing
Literature:
Grendel
Captain Nemo
Prof. Moriarty
The Grinch
Shere Khan
Smaug
Television:
Angelus
Xena (she started as a villain, for those who don't remember)
Eric Cartman
Dr. Zachary Smith
Cancer Man aka Cigarette Smoking Man
Montgomery Burns
Endora
Video Games:
Donkey Kong
Carmen Sandiego
Scorpion and/or Sub-Zero
Psycho Mantis
GLaDOS
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Classic!
The only ones I'd add to those already mentioned in this thread are the Daleks, Norman Bates, Dracula (the novel version please) and Annie Wilkes.
If we can choose historical figures I'd add some more.
Al B.
