Your favorite main antagonists from anything fiction

[Che]

Those 11 still are in Video games.

You're correct, but the topic states it can be from any fiction.

I'm gonna go with:

Samuel L. Jackson in Unbreakable, Agent Smith from the Matrix, Vincent from Collateral, Sephiroth from Final Fantasy VII, The Joker from Batman(1989), and The Joker from Batman: Arkham Asylum (Mark Hamill).

I can't think of any others at the moment, perhaps I shall edit this later.