It isn't just Marvel.
Batman and Batman Returns were good movies, then Batman Forever ruined the pattern.
Superman and Superman 2 were also pretty good, but then Superman 3 was terrible.
They should cast me as the next villain. I'd kick his ass.
The opnly villians I remember from Spiderman were Hobgoblin and Doc Oc and Venom.
The others from the comic were
Kingpin Carnage Lizard Mysterio Rhino Kraven the Hunter Chameleon Shocker Electro Tombstone
Batman Three sucked?
Two Face and The Riddler? You didnt like Jim Carrey as The Riddler?
Jim Carrey was great. His style fits the riddler perfectly.
I didn't like the movie because it was geared more towards children, whereas Batman/Returns were less childish (stylistic yes, but not childish) and more Dark an atmosphere. Let alone that was a terrible terrible Two-Face.
I think of any of the Spiderman villains not yet used, Electro, Lizard and Carnage are probably the best choices.
Spiderman doesn't have a very good rogues gallery, IMO.