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And the required example: "What You Feel", by the dancing demon Sweet in the Buffy the Vampire Slayer Musical Episode "Once More With Feeling".
: The Master singing Doctor Who Scissor Sisters' "I Can't Decide" at the Doctor. "Oh, I could throw you in a lake, feed you poisoned birthday cake. I can't deny, I'm gonna miss you when you're gone..."
And of course, "Voodoo Child" from the episode before. "Here come the drums, here come the drums..."
has "The Hitcher" and "Eels".
The Mighty Boosh Also arguably Old Gregg's "Love games". He's not exactly a villain but then again there is what he did to Curly Jefferson...
And what he plans to do to poor Howard
The Lallakki song Kill the Humans in BBC series Hyperdrive.
Averted in with the Nightman's cut song It's Always Sunny in Philadelphia It's Nature, Shit Happens from "The Nightman Cometh. While the song is the Nightman's major piece, he spends it justifying his deeds by claiming to be evil by nature ("Some people are born evil with the eyes of a cat").
has a few examples: Super Sentai Himitsu Sentai Goranger has Akuma no Kurojuujigun, JAKQ Dengekitai has "Iron Claw's theme", Kousoku Sentai Turboranger has Oola no Urami, Kyoryu Sentai Zyuranger has Bandora's theme, "Dolla! Theme of Witch Bandora". And compare the opening theme to Gekisou Sentai Carranger ( seen here) with the theme song to of that series, The Psycho Rangers Bousou Sentai Zokuranger ( here).
Kamen Rider Gaoh is so much of a Bad Ass that he gets his own solo for his fight theme song of which all of the others are duets. Despite being included on The Movie's soundtrack, it is too good for the theatrical release and only gets played in the Director's Cut.
All of Kamen Rider Kiva's members of the Checkmate Four have their own theme song. All of them, including the two Queens and two Kings (if you count Roots of the King as such).
In Robbie Rotten gets quite a few of these. Most notable examples include LazyTown Master of Disguise, Good To Be Bad, Woof Woof Woof, and Fun To Be The Mayor.
Does the infamous YOU ARE A PIRATE count?
Then there's Versti Fantur (Worst Villain) from one of the original LazyTown plays, which is arguably creepier and more sinister than it's remade counterpart "Master of Disguise".
The direct-to-video show had the grinch-like Cavity Goon, who got his own song The Adventures Of Timmythe Tooth here (NOTE: Despite the video's title, these are not the Muppets).
The Showa Kamen Riders have many. "Oh Shocker!" and "Akuma no Shocker" for the original, "Destron Sanka" for Kamen Rider V3, "GOD(Government of Darkness)'s March", ( Kamen Rider X) and "Wahhaha! Terrorizing The Country!" for Kamen Rider Stronger. The last two are done by Names to Know in Anime Koorogi '73.
The Muppet adaptation of " The Frog Prince" has Sweetums' self titled song.
has the Riverbottom Nightmare Band singing an eponymous song. Lyrics include "We don't brush our teeth, 'cuz a toothache can help us stay mean" and "We break up your place / We are dangerous when we are near". The song actually fits into the plot because it is an entry in the local Emmet Otter's Jug-Band Christmas Talent Contest.
The short-lived had one song in particular called Cop Rock "Baby Merchant" that fit the bill.
While he's not technically a villain, the Janitor's verse in the middle of Dr. Cox's Rant Song certainly counts.
One Saturday Night Live "TV Funhouse" sketch had a fake preview for "Titey", a animated Titanic film produced by Disney. The villainous iceberg (voiced by Whoopi Goldberg) apparently gets her own villain song.
has many of these. Just as an example, Horrible Histories Caligula, Elagabalus, Commodus, and Nero trying to prove which of them was the baddest Roman Emperor. And the winner is... Nero!. Other highlights include:
The Annoying Orange tv show had Musical Nightmare Sung by Teddy Juicer.
has " Game of Thrones The Rains of Castamere" for Lord Tywin Lannister, and it is . See also awesome the metal cover.
has Fraggle Rock sung by Wander McMooch.
Manic McMooch even has one of these in the Season 5 premiere, 'Tough Boys', appropriately called the MacGyver Tough Boys Rap. Of course, it only works if you believe the Tough Boys are the episode's Designated Villains, because they're just vigilantes trying to end their neighborhood's crack problem. Nevertheless, the song sounds pretty cool.
In the category of "not sung by the villain" is Black Adder's title song, which has many variations throughout the life of the series and associated specials. The lyrics both praise and lambaste the titular Villain Protagonist.