Hmm... Here's what I think:
The DS would be extremely difficult to emulate at full speed on the PSP, because of the two processors.
Nintendo cretated an N64 emulator for their Gamecube, and it worked at fullspeed, yes... but even still, it had some frame rate issues in games (think Majora's Mask in Zelda Collector's Edition). The Gamecube's 485 MHz CPU with its 162 MHz GPU, compare it to the PSP's 333 MHz CPU and its 166 MHz GPU. But then again, it was running in 640x480 as opposed to the N64's 320x240...
The PSP could very well do N64 emulation at full speed, but the DS has two processors: the 67 MHz ARM9, and the ARM7, the same processor used in the Game Boy Advance (GBA's ARM7 is 16.8 MHz while DS's ARM7 is 33 MHz). So, essentially, you are talking about emulating a double-speed Game Boy Advance and an N64 at the same time, for the most part.
Another thing that the second poster pointed out is that the N64's processor and the PSP's processor are similar, so emulation could be made faster.
By the way, processor speed numbers, I got from Wikipedia, even PSP ones, just to confirm everything. It seems they say N64 speed is 92.5 MHz, compared to the original post's 62.5 MHz...
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