Hmm...can only really think of video game soundtracks. And Black Hawk Down. Don't know if these two really count, but since both are played when the Bad Guys are killing a bunch of innocents, I guess it sort of counts.
Dr. Facilier's Friends on the Other Side comes in close second, but my all-time favourite has to be Dimentio's The Ultimate Show... Granted, it's technically not a villain song, but who cares, it's great.
"Outfox the Fox", from the classic Danny Kaye movie "The Court Jester".
I don't really know if this qualifies, as the Black Fox is actually a heroic character, but since he is an outlaw trying to overthrow a king, and the song itself might just as well have been performed by a villain, I'll take my chances.
How could I not? I played through this very game again about two weeks ago (first time in 3 years), and fighting Starscream, Cyclonus and Tidalwave rocked harder than ever - both the battles and the music!
Besides, even though it's short, Starscream has one of the best boss battle intros I know of.
Not necessarily a song, but I also like the "why so serious" theme from The Dark Knight. Everytime the Joker was about to do something, there was a note played by stings and horns that would get louder and louder until something happened that was really fucked up.
I too have soft spots in my heart for Dancing Mad (FF3/VI Kefka's theme), Sweet Transvestite, and Mark Hammel singing Jingle Bell's/Batman Smells as the Joker. But although I like One Wing Angel, I've always preferred JENOVA absolute.
Seriuosly though, only two posts for Chrono Trigger: The Battle With Magus?
And I'm the first one to post: FFX: Other World (First CG movie and first part of Final Boss)?
I also have a nostalgic soft spot for DQ/DWIV: Necrosaro's theme and Xenogears "The One Who Is Torn Apart" (Id's Theme) and "Awakening" (Fight With Deus) are two more awesome songs from Chrono Trigger composer Yasunori Mitsuda.
Since the best songs, (Hellfire, Be Prepared, and such) all are already posted, I will try a bit more obscre ones or ignored ones.
It's Our Secret of Our Survivial: Even though this was put into a very stupid, very wierd film, this song really is threatening. A group of Moles sing about how the survive in the world, what a dark place it is, all with a song that sound like a heart beat.
http://www.youtube.com/watch?v=sy62mqmqwCQ
Poor Unfortunate Souls: A very risky song in the first disney princess film ever. Ursula sings a convincing song that she is the only one who can bring happiness to "Poor Unfortunate Souls," and how she can easily get Arial her man. She even goes into how men are all lustful idiots that don't care about personality at all. Really, look at the video and you will see.
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