Composed by Murray Gold, "My Angel Put the Devil in Me" was the third original song commissioned for the revived Doctor Who series and the first to not be connected with one of the Christmas specials. It was the first of these songs to be actually performed on screen. Actress Miranda Raison, who portrayed Tallulah in the episode, sang the version that appears in the episode. Later, when Gold expanded the song into a full-length version for the Third Series soundtrack CD, Yamit Mamo was hired to record that version.
Raison's performance marks the first time an original song was actually shown being performed on screen in Doctor Who.