Of All Time? If you can get your hands on some of the Marvel Masterworks books featuring early Spider-Man, Avengers, FF etc. then that would give you a great introduction to the background and the characters you now enjoy.
Then if you can get any of the Wein/ Cockrum and Claremont / Byrne X-men series culminating in the Dark Phoenix Saga (These were late 70's early 80's). Also Millar had a great Daredevil run in the mid - late 1980's.
Company Cross overs were big in the 1990's so I would recommend Marvel Vs DC and Avengers Vs JLA.
More recently what people above have said, plus TPB's like House of M, Secret Invasion and Civil War
Enjoy
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