I have playlists for my characters, so yes. But I'll keep it brief.
The comic's perfect song is from Persona Q2, Road Less Taken, which is just the perfect mood and even lyrics for it. I caught it while looking for inspirations for the comic, and I can see the anime opening play in front of me if I'm listening to it.
As for the main character, Mortimer, I have a lot of general mood songs in his playlist for illustration, but the one that most perfectly encapsulates everything about him would be Out of Tartarus from Hades. Both a strange, calm start, going into a driving action version of the same melody that really shows him as a chill but intimidating character with terrifying potential if angered - or desperate - enough, always with a strange atmosphere.