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In the webcomic Narbonic, mad scientist Dr. Lupin "Wolf" Madblood and his 15,000 robot duplicates spend a week of strips singing the "Madblood Battle Anthem".
In an in-comic example, Jason of Something Positive asks Davan to play Judas Iscariot in his deliberately provocative play, Nailed! Davan's big musical number is called "You're The Son Of God, But I'm A Son Of A Bitch".
Although mostly lyric-less, Homestuck's main villain proper, Jack Noir, has the very catchy and uptempo theme song - Black, which starts off slow and simple, then builds into a grand production.
The Good Witch has "Things Will be Different." This is a rather unusual Villain Song in that it is both very upbeat and sung by the comic's protagonist. (Justified since she's a Villain Protagonist.) The song focuses on Angel's happiness that she is free from her previous life as a transsexual male who was ostracized by everyone in the town, and how great life will be now that she has infinite power. Which is to say, great for her, as she is also ruining the lives of everyone else. Throughout the song, she carelessly transforms innocent bystanders into random and bizarre things, and hypnotizes the others into singing with her. Ultimately, it foreshadows the selfish and arrogant bitch she'll eventually become.