I've been thinking about this for a while, and I think that these are crossovers that have YET to be tackled. Plus they could probably offer some lucky newbie his first fanfic plot:
SPIDER-MAN: The Ghostbusters and Spiderman team up to stop both an ectoplasmic being and one of Spidey's villains. Maybe Master Spider would be interested in this.
DRAGON BALL Z: If Ectodude can make posts about a Sailor Moon-GB crossover, then DBZ has options too, if you've seen the series.
MEN IN BLACK: A secret AlienBusting agency and the Ghostbusters teaming up. What are the Odds of the outcome?
PHANTOM INVESTIGATORS: Everyone here at the site hates this series SOOOO much. Why take out the series in a story where they can't handle a major ghost (not one of those pansywaists they have fought so far) and have to call in the pros: the Real Ghostbusters.
X-MEN/X-MEN EVOLUTION: Either would work.
BATMAN: Another hero of NYC.
SEPT 11.: I think it would be a good thing to see the horror of 9/11 through the eyes of a GB.
This list is only half done. If anybody is willing to do this, contact me and I will gladly give aid.