Let's see, for the first few years, they reused Dr. Doom every six to eight issues. Other than him, there are the Skrulls, the Sub-Mariner, the Impossible Man, the Frightful Four, the Mole Man and his mole people, the Puppet Master, the Mad Thinker and his awesome android, Diablo (a sorceror with the Philosopher's stone, which can transform matter), the Molecule Man, and Galactus.
I'm thinking that of the regular recurring villains, the Skrulls could work. A reworking of their first appearance could work. They imitate the Fantastic Four to discredit them as a method of preparing Earth for invasion. Movie makers love having people imitating others, and having skrulls, shapefhifters, makes for a bunch of good possibilities.
Or maybe go with two villains, skrulls and the Puppet Master. The Sub-Mariner could work, but they may want to save him to use as a good guy later on.
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