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I'd probably go with SNES to N64 just because of the big move to polygonal graphics combined with having something on the level of Super Mario 64 day one. However, just comparing the system's 2D advancements over the SNES wasn't nearly as big of a jump for me as NES to SNES or N64 to Gamecube.

Every Playstation jump was substantial too until PS3 to PS4, and Saturn to Dreamcast was also huge.