git currently requires that any file it manipulates get mmapped, this limits the file size to your memory size.
git's pack file format uses 32 bit offsets, which limits the largest pack size to ~4G (I believe it uses unsigned 32 bit values, if it's signed values then the limit is 2G) I think that it is always pointing to the beginning of a file, so a file larger than 4G can exist in a pack, but would be the only thing in the pack.