Drawn to Life and Drawn to Life: The Next Chapter had fantastic soundtracks. They weren't giant, epic orchestras or anything, but what power the DS had for music was taken full advantage of. Catchy video game music at it's finest.
My favorites are "Ooh, Wilfre!" (the villain's theme) and the final boss theme. The main theme is pretty great as well. The levels all have memorably catchy tunes, and the original songs at the end to both games made me cry.