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I'm unfamiliar with the innards of these systems, but a brief overview shows the 3DS  has 2/4 times as much RAM, (depending on PSP model) twice as much VRAM, and while its main screen is lower resolution at 240x400 vs 272x480 on PSP, 3D pushes the number to 240x800, plus there's the 240x320 bottom screen.

As far as how the CPUs and GPUs compare though, I'm at a loss, can anyone tech-savvy explain to me how they compare?