I am using some unmanaged code that is returning pointers (IntPtr) to large image objects. I use the references but after I am finished with the images, I need to free that
It depends. Do you have any documentation (or source code) for the native functions you are calling?
Native code doesn't have a single deallocation function. This is one of the great advantages of the CLR.
If I was a betting man, I'd go for GlobalFree. But it's not going to be much fun trying various APIs until your code stops crashing.