For Spider-Man, I still think the old Lee/Ditko books from the '60's have yet to be topped. The "Essential Spider-Man" books reprint huge chunks of them, but sadly they're in black and white.
For X-Men, many people swear by the Claremont/Byrne era. While this is certainly the time period that made the X-Men what they are today, I find that the writing style hasn't aged well (and unlike Stan Lee's stuff, it doesn't have a retro-fun feel to it either). Still, you could do a lot worse than "The Dark Phoenix Saga," which has a lot of defining moments for the classic X-Men characters. For a more modern take, I recommend Grant Morrisson's "New X-Men" series. Trade paperbacks are numbered on the spine for easy chronological reference.
If you do feel like branching out a bit, while staying in the super-hero realm, "Watchmen" is the way to go. It's generally considered the best super-hero story of the modern era (if not the best ever) by the best comics writer of the modern era (and artist Dave Gibbons is hardly a slouch).
Have fun!
sk
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"If I could have one wish, as in the fairy tales, I would unmake my past, and rise like Lazarus and stand in sunlight and banish all the dark."
D. Tibet
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