I was just browsing last night and stumbled across a 'Mob Psycho 100'/'Scooby-Doo' fusion that has absolutely no business being as good as it is. The author framed the entire Mystery Inc. gang as low-level espers who investigate paranormal cold cases, with Shigeo as their reluctant, hyper-powerful consultant. The tonal clash writes itself—Scooby-Doo's goofy, formulaic mysteries crashing into Mob's quiet melancholy. It shouldn't gel, but the fic nails the character voices, especially Reigen as a hilariously inept fake medium the gang keeps running into.
What makes these weird crossovers work, I think, is how they force 'Mob' characters into genres they'd never belong in. Another one I saved pairs the series with 'The Magnus Archives', casting Mob as an Archive assistant who is completely immune to fear-based entity manifestation. The horror elements get subverted because the most terrifying beings just... can't affect him. He's a calm spot in a cosmic horror narrative, which creates this amazing tension. You end up focusing on how the other characters react to his unnatural peace, rather than on the scares themselves.
Those are the stories that stick with me—the ones that use the crossover to highlight something fundamental about Mob's character that the original show only hints at.