ASM 2 is hard to beat! That was an incredible live action suit!
This is going to sound silly but...
IMO, the 3 best live action suits were probably:
ELECTRIC COMPANY SPIDER-MAN
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The SPIDER-MAN ATARI VIDEO GAME AD suit from the commercials.
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And the 90's REGISTER TO VOTE PSA AD... that one might be the best one ever! ;-)
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Special mentions to the 70's live action suit with it's outside the suit web-shooter and utility belt, and those wonderfully wonky eyes.
And to the live action Japanese TV Spider-Man!