i had a similar idea to this a while back. you could buy up spare battery compartments, and what i would do then is mold something like the bottom half of a game controller, with the L2 and R2 buttons on it. this would go around the whole bottom of the console to give a more comfortable and less square grip along with those buttons. the whole unit would connect via usb for the switches, so no internal modding. a usb hub could be added, possibly along with some kind of 3G dongle, inside the hand grips, maybe some additional storage, which would all connect to the USB hub. it wouldnt be the most on the go friendly setup, but it would make it more comfortable for more intensive gaming times.
the logistics of it all though is a little complicated though, getting the perfect shape and getting it made.