Avengers 6 and 7 J Buscema, addition of the Black Panther and the Vision
Fantastic Four 5 and 6, first appearances of the Inhumans, Black Panther, and Galactus, Silver Surfer
Silver Surfer 1, J Buscema and Stan Lee
Uncanny Xmen 2 and 3, Byrne and Claremont
Xmen 6 Neal AdamsĀ 
Thor 4 and 7 Kirby greatness

over the limit but very worthy

Captain America 3 Kirby and Steranko but a few weak stories involving a villian with a bad french accent and a villian with a paste gun
Nick Fury 1 Steranko and Kirby and no need for superpowers in these spy stories
Warlock 2 Starlin, I don't love this as much as Captain Marvel Starlin which I don't have yet
Thor 5, 6 Kirby Thor has become one of my favorites

I only have a collection of 24 volumes so far, but these are the best