Okay, back on topic.
One thing that worked very well for my chapter was inviting NPHC or MCGC orgs to join our homecoming float. Campus rules allowed up to 4 orgs, but most Greek floats were on CPH sorority and one IFC fraternity. Groups from the other councils were traditionally much smaller, and couldn't do a float on their own.
For them, it meant a chance to participate in a campus-wide activity that they didn't have the people/resources to do alone. For us, it meant we got to hang out with some new people (admittedly, we were most interested in the male people).
Obviously homecoming floats are the right activity for every campus, but you should take a look at what you already do that may interest groups from the other councils, as well as what you'd like to get out of a relationship with some of those groups. If you can find common interests, great. If you find that doing something with another council makes about as much sense as co-programming with the rugby team, don't bother.
(One exception would be those huge displays of Greek unity that you don't even want to do for your own council, but do for show, i.e. groundbreaking on a new house, installation of a chapter. You should do those for any chapter on your campus, regardless of council.)
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