I’m surprised nobody’s mentioned Schubert’s Erlkönig. Chuck Jones used that for “evil” music in at least one Bugs Bunny cartoon.
Second to “Night On Bald Mountain”. Also “Ride Of The Valkyries”. My favorite, though, is the “witch music” played in “The Wizard of Oz”. I used to hum that every time I saw my boss approaching.
Good suggestions all.
But As Voodoo Lou noted, the songs that create the worst feelings during death and destruction are songs that aren’t oriented that way - The Andy Griffith theme and the Liberty Bell March were also mentioned.
Therefore, when I unleash my firestorm of humility upon the world, the songs will be more along the lines of:
“Lucky star” - Madonna
Liberty bell March (great suggestion, Scuba Ben. I will spare you)
Let the Good Times Roll -the Cars
Oh! You Pretty Things -David Bowie
New Day Rising - Husker Du
Sam - the Meat Puppets
Girlfriend - Matthew Sweet
memphis, Egypt - the Mekons
whole Day Off- Oingo Boingo
Life begins at the Hop - XTC
and wind it all up with
Good Feeling - Violent Femmes.
OK then
“Get Out of My House” by Kate Bush (more the music than the lyrics)
Pretty much any Nick Cave song, but especially “Mercy Seat”
“London Calling” by The Clash
“Lady Cab Driver” by Prince (especially the sex bit)
A few years ago, a law student here flipped-out and smashed one of the glass display cases with her walking stick, THEN she sat down with her boom-box and played Kermit the Frog’s “Rainbow Connection” loudly and repeatedly until the cops came for her. Imagine THAT song while glass is flying.
Anything Can Be Made Evil,
Patty
Sam Sham and the Pharoahs’ “Little Red Riding Hood”
waitwaitwait… I got it. the best soundtrack for EEeevil:
Metal Machine Music.
Hahahaha!
Are you the same voodoo lou who sells dolls and spellbooks? I think my love doll is missing it’s mojo.
Anyways if I was the supervillian I’d probably use Devil went to Georgia.
Although Money and Meeskite from Cabaret would be interesting too. Maybe some not-total-sinister-lighter-side-of-evil themes.
For that silent except for soundtrack battle montage, when we see the hero vanquished and all his plans coming to ruin?
Rainbow Connection by Kermit the Frog
'cause I’m evil, and nothing will make my triumph more complete than it occuring to that song.
I mean color me once by the violent femmes? You’d expect me to win while that song is playing. 
CC
Haha, that’s not me, but a friend got me a “Voodoo Lou” voodoo kit as a gift! I borrowed the name from the swing band Big Bad Voodoo Daddy back when I was playing sax in bands and DJ-ing swing dances in the late '90s, and it stuck. (I am Lou, though.)
Bide your time…
Let them come to you…
Wait for the perfect opportunity…
Unleash Hell
Careful With That Axe Eugene Pink Floyd
Forgot this one yesterday:
Blue Oyster Cult: The Reaper
Good call, vsquist! I’d also add
Blue Oyster Cult: Godzilla, Career of Evil, Hot Rails to Hell and Black Blade
Bauhaus: Bela Lugosi’s Dead, Terror Couple Kill Colonel
Killing Joke: Wardance
ELO: Fire on High
yet another vote for Moussorgsky’s Night on Bald Mountain
George Crumb’s Black Angels.
Mr. Bungle - None Of Them Knew They Were Robots
red riding hood creeps me out
for when things blow up-that song with the cannons… the one the army tattoo always plays!!
for car chases- sunshine lollypops…
general- the guitar from little acorns by the white stripes
for brainwashing- relax by franky goes to hollywood… well it worked in Zoolander!!
“He’s got the whole world”
It worked in ConAir where Steve Buscemi’s character (nasty serial killer) starts singing it as he’s covered with blood of the last victims and the plane he’s in is going down.
It worked for me anyway.
Massive Attack’s “Angel” - nice ominous tune for the final destruction, or maybe when the supervillain betrays the one who was supposed to be his (her) true love and the only hope for stopping him (or when the sv kills the hero/hero’s true love).
the various music from the pc game Alice.
I’d have to offer “Psycho Killer” by the Talking Heads for the tightly wound axe murder types.
Pretty much anything by the Cramps for the giggling psychopaths, although Screamin’ Jay Hawkins is another great (hats off to Pez).
My personal favorite for the ultra-sinister, criminal mastermind has to be “The Adversary” from Crime and the City Solution (lyrics)
Indeed, this song (like most of Who’s Next) comes from Pete Townshend’s ill-fated rock opera Lifehouse, where it was supposed to be sung by the villain of the piece.
I may be perverse, but for some reason the Beatles’ “Being for the Benefit of Mr. Kite” would work pretty well for supervillainy, even if you don’t want to cultivate a Jokeresque Evil Clown persona… 