I don't really have much confidence in it... the main CPU is a huge burden, and synchronizing the two would be a pain (they share fast, cacheless memory). The video alone is at least 2x as demanding, but probably often more (especially with 3D). You could perhaps put the sub-screen on really high frameskip.
I don't really know what DS game code is like either, IE how much it pushes the CPUs. Since it has instruction cache it might be that proportionally more code on the ARM9 is ARM rather than Thumb (unlike GBA), which means more work in emulating. And the memory emulation would probably be more complex because the memory subsystem is more complex. I can get some average load games to use about 5ms per frame on PSP - multiply that by 4 and it's 20ms, way above the 16.7ms per frame you need to be fullspeed and with nothing left over for graphics. Don't even want to mention the heavy load games (urgh, FF6)
gpSP's speed isn't always maxing out the PSP, but a lot of the time it could definitely use a more free CPU time. It's not that it's 100% optimal but I personally only know of so many ways to make it faster, and not an awful lot faster.
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