It would have to be something that would fit all of their niches: A bad nostalgic movie that is also a comic book adaptation. It needs to have a bad current game attached to it as well as a terrible old game attached to it. There is only two franchises that could be used, Spiderman and Superman. Both were in bad movies, bad video games old and new, and both had bad comic book stories written about him.
Too bad there is already the Nostalgia Critic video, as well as a Video Game Nerd one, devoted to a Superman tie in. Spiderman could work, the retro 70's tv series and the made for tv movie from the same time.
Well, Nostalgia critic does things post 2000, so he is not going to do a Superman Returns or a Spiderman 3 critique.