I think the only real competition is Killmonger. And maybe it's because I read a lot more Spider-Man comics than Black Panther, particularly many that focused on Mysterio. Or maybe it's because I think Mysterio is more "comic-y" than someone like Killmonger in general. But I left FFH absolutely giddy with his portrayal in the movie. He completely made that movie. Unlike many Marvel movies where the villains are pretty whatever, I feel the movie would have been extremely lackluster without the focus on him.
I really just don't see how they could have done him better at all. They straight up ripped him from the comics and put him on the screen. From the entire movie being based around his deception, to him actually seeming and the marketing pushing him being a good guy for people that didn't know, (my girlfriend legit thought he was a good guy. The revelation was huge to her while also satisfying to fans that already knew), to one of the coolest moments in MCU history in the warehouse with Peter.
And Gyllenhaal did an incredible job. While I've never thought he was a bad actor at all, I guess I just always saw him as someone with middling range. But he destroyed Beck. Absolutely nailed it. He was able to switch when he needed to switch, look heroic when he needed to look heroic, and break down when he needed to break down.
Not to mention the character was dropped at not only the perfect time during the MCU, but in the real world. Where truth is very much something to actually be manipulated.
As far as Thanos....MCU Thanos was wonderful....as an end boss. But I don't think he was as well realized straight from the comics as Mysterio was. (Not saying I don't appreciate his changes though).
This is of course not including non-MCU villains, like Magneto and god damn Norman Osborne. Willam Dafoe's Osborne imo is the greatest Marvel villain to ever be realized on screen. (Yeah the mask sucks but wtf ever, every other single thing makes up for it).
Not to mention he's one of the few villains that seemingly are going to have a lasting impact, considering his possible final broadcast
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