Spider-Man is probably the most straight forwardly good one, but I've always loved Batman's crazy level of ambition, I really, really miss when blockbusters would have that kind of pop surrealism.
Superman paved the way and Reeve was the best cast, there's a difference between a good actor cast in the role and a guy who truly feels like he simply embodies the character, but there's some odd aspects the script, making the world go backwards reverses time? But it works in a child fantasy logic sort of way.
It's a tough choice, but I would pick Spider-Man.