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In comics, I always answer Doctor Octopus.
(NB : I use the moniker of Grey Gargoyle because he is one of the few French characters of the Marvel Universe and because I like the Gargoyles cartoon).
In all of fiction, there is no name that immediately comes to mind.
Among the ones that I like in movies : Nosferatu, Joker (Nicholson & Ledger), Dracula (Coppola), the Strangers of Dark City, the Cenobites of Hellraiser, the Xenomorph, ...
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The Cenobites weren't really villains though, were they? They were explorers in the dimension of pain and desire. Kirsty was able to reason with them the 3 times they crossed paths (movie 1, 2 and 6). Everyone else got on their bad side by messing with the status quo.