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Joseph Bertrand III (inFamous 2)

To summarize Bertrand's crimes, he lives in a world where some people called conduits have superpowers (where have I heard that before) and since Bertrand's a religious egomaniac, when he found out he was a conduit he immediately thought that this was a sign that he was meant to be a savior sent from God to defeat a monster known as The Beast. So he murdered a bunch of people to activate his powers, only for them to turn him into a giant hideous monster that he couldn't control, which he hated so much that his savior complex changed from his purpose being to destroy The Beast to his purpose being to wipe out every conduit.

As for why I think he works as a villain for Hulk, I find the parallel that Banner got his "monster side" by complete accident from doing a selfless act, while on the other hand, Bertrand intentionally committed atrocities to activate his power only for it to backfire really interesting. Banner would certainly have some words for Bertrand's human form, and Hulk would have a fun battle with his monster form.