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I've always liked Loki from the Marvel films.
Really dig his character as a villain who isn't super cliche and edgy but more playful and mischievous.
EDIT: Forgot to mention Handsome Jack from Borderlands 2. They guy was seriously a funny asshole and I had way too much fun killing him.
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Agreed on handsome jack
But I would also have to say the dude from Far Cry 3 (what was his name?) --
"Have I ever told you the definition of insanity?" I think his character was perfect.