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...Dr. Robotnik (both Sonic cartoons; one's a bumbling fool, and the other has ice in his veins).
The Joker always had the best jokes.
Wile E. Coyote, Suuuuper Genius.
Dr. Heinz Doofenshmirtz (Yes, I watch way too much kiddie TV...)
With some Final Fantasy villains already mentioned, there is one name that has to be included...Kefka.