I am still pretty sure you would not need the full number of pins. It would make it easier to do if you had that, but as long as you have an adapter it could still work. Would probably need a more advanced adapter though since I suspect when the Pi is used for the PiStorm much of the work is done on the Pi.
It could be very interesting if it was possible to just connect a 68K CPU through an adapter, but if a Pi was connected, it would be more useful I think.
Another thing though, is that if a Pi, to be used as a PiStorm, should be connected to the MiSTer, it would probably have to be the GPIO that the RAM uses right now. At least I am pretty sure that is what the SD RAM is connected to. The GPIOs are not the same speed, one is 10mhz the other is 50mhz, and the 10mhz one is meant to be used for IO stuff. So that must be what the analog IO boards use. It could be nice if there could be made some hardware switch, that would allow to connect several things to the GPIO on the MiSTer, and let the cores somehow set which of the connected things would be used. That would make it a lot bigger though, so it probably would make more sense to just reconfigure it physically connecting what you wanted to use the MiSTer for.
But maybe a Pi connected to the SD RAM GPIO could also be used for SD RAM, emulating the SD RAM. But that might cause timing issues and such. I guess it could solve the RAM timing issues of hybrid cores though, if the SD RAM and the CPU is done on the Pi. But it would probably also further bottleneck the whole solution.