The intro song for Despicable Me is one of the most fantastic villain songs ever. It’s like a twisted upbeat version of a James Bond theme. Also it’s amazingly ear-wormy.
For nastiest? I have to say Ursula’s “Poor Unfortunate Things” always gets me creeped out. She’s just so nasty about it!
For non-theatrical-release villains, GlaDOS’ ending song in Portal. Very nice. “we do what we must, because we can.” Such a good song.
I came in to mention this song. I sing it more often than is probably healthy, and I’m toying with a script for a musical adventure that will allow me to inflict it on hapless players. Definitely a theme song for a cheerful, willfully malicious villain.
Still Alive is also a great villain song. I’m torn between it and the Imperial March. I love both, but for such utterly different reasons that I’m unable to weigh one against the other.
Oooh, I just thought of a good one: The theme from Halloween for Michael Myers.
Mussorgsky’s Night on Bald Mountain as used in Fantasia.
If you aspire to be Evil Incarnate, THIS is the type of theme song you want!
The first and only one that came to mind was the great music Rosza wrote for the 1946 version of “The Killers” (not the 1964 one, which is also awesome). Couldn’t find a good YouTube of just the exact moment when “you know” when “it’s” going to “happen” – DON’T.
I like her song from the sequel (spoilers for Portal 2, obviously). It helps that Jonathan Coulton was able to write this song with the actress’s singing range in mind, as opposed to “Still Alive” which he wrote ahead of time. Still, neither one is really a “theme song” for her, I think. Or at least, not a Leitmotif, as the Imperial March is for Darth Vader.
I’m also fond of the Klingons’ theme from the Star Trek movies (it of course also becomes their heroic theme from time to time on TNG, when they are allies with the Federation).
For several hours yesterday I tried to find a YouTube clip that would have enough of that little “dahn-dahn-dahnnan-dahn” thing that I could point to it and say “that’s it” – all with no luck so far. But I did find some things that make me a little ashamed to say that I don’t know all that much about Native American music.
Despite this being off-topic of the current thread, maybe it will strike others the way it has me: Native American Indian Spiritual Music - Ceremony to Mother Earth.
I haven’t given up trying to find that little whatever-it-is.
I instantly got the Cruella de Vil song from 101 Dalmatians in my head. How many villians have a song about themselves?
What about the strange whoosh/hiss/swoosh/wheeze/whatever noise in Friday the 13th? Does that count as a theme?
Goldfinger. I can’t think of another Bond villain with as memorable a theme
There’s the Man With the Golden Gun. I’m partial to that one as it’s a bit more upbeat.
I also like the Saruman/Isengard theme from the Lord of the Rings movies, with that heavy syncopated drumbeat.
I actually like this song better than “Still Alive” - as I believe I mentioned in another thread, I think it works fantastically as a breakup song for a bad relationship. A really, really bad relationship.
It’s not specifically a villain theme song, but I pretty strongly associate the opening of “Tubular Bells” with Bad Stuff Going Down.
The music from David Warner’s pocket watch in Time After Time.
Except that just as often, that piece indicates that the Good Guys are about to Kick Some Ass, as in its first documented appearence in a major motion picture.
Dr. Horrible had some kick-ass songs he sung.
Good point. I was thinking more of The Omen soundalike and how that piece is even used as motivational music at football games! Same with the Darth Vader thing.
I know there must be other “theme songs” for Satan and other demons but I’m having trouble remembering the specifics. The Exorcist and The Omen are closely related in my mind’s ear. 
Everybody knows the Wicked Witch of the West’s theme!
“The Great Race”. Professor Fate. Push the button, Max
darth vader? the shark? nah. brutus’ entry into any popeye scene always changes the whole mood for that day.