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Can't speak for PSX, but I know for sure that not all N64 titles were designed to run at 60FPS at all times. The console is simply not powerful enough to do this with all games. NTSC Ocarina of Time runs at 20FPS in-game for example. A few games such as F-Zero X had severe graphical and sound trade-offs/optimisations to maintain 60FPS in-game. The Perfect Dark and Goldeneye engines are designed with a variable frame rate rather than a fixed one.
There is nothing you can do to improve emulated framerate beyond the abilities of the target system.
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