Pattinson already has that "weird" vibe, like Gosling or Gyllenhaal, or Mat Smith, or David Tennant, or Hugo Weaving, or Michael Sheen, or Joseph Gordon-Levitt, to name a few. There's no problem with one single "weird" actor. Pairing two or more with that same vibe, it only works if you're doing dark comedy. You need balance, the weird one and the serious one.
Now see, that's something I hadn't thought of....
And you're right. Pattinson was perfect as the slightly quirky but efficient partner, teaming with another weird one would have taken away from the tone of the movie.
Oh man, I just thought about it... Gerard Butler!
Daniel Craig -- you're right, is an absolute buffoon in real life -- is still my top choice. I think he would have really fit the smart-enough-to-understand-quantum-entanglement elements but still gruff enough to carry out the physical action. But second to Craig, I would have definitely enjoyed seeing Butler in the role.
I don't think Gerard Butler could convincingly play a guy who gets the quantum-physics of the matter, but I feel like he would be the straight man just brash enough to get keyed into how things work through Pattinson, and basically go full-bore action hero to solve the situation. Also, I could have totally believed someone like Butler was ex-CIA; brash but good at his job.
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