I really adore ... quite a few. Sigh.
Alan Rickman's Sheriff of Nottingham has to get a mention. Prince of Thieves is in many ways a dreadful film, but Rickman and Freeman are gods and save it. Of course Alan Rickman also played Hans Gruber. The guy is one of the best villain actors out there. I haven't seen the Harry Potter films but he's probably great in them too.
Bela Lugosi's Dracula is best Dracula. However part of the reason why he's the best is because he's so damn good you sorta wish the vampire would win. So he doesn't really come off as a villain.
However I think my vote would have to be for Goldfinger. Except there's no James Bond in the list, you nut.
"Do you expect me to talk, Goldfinger?"
"No, Mr. Bond. I expect you to die!"
He was terrific.