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Pitt as Galt would work, but from what little I have seen of Jolie, she hasn't the depth of Dagny. The real question for me is who they will cast as d'Anconia.
I pictured Galt as looking a bit like Robert Duval when I read the book. Not sure why. Dagny looked like Rand, which made the sex scenes a little icky.
d'Anconia would be a wonderful chance for Sasha Baron Cohen to try out a new fake accent.