I picked the Skyfall PTS just because it features so many stunts and finally feels like Craig is James Bond (that scene where he jumps from the crane onto the carriage and casually walks through the car!)
Overall, I voted for Quantum of Solace just because every action scene in it is so brutal. The only action piece in it where I don't feel danger is the Bolivian plane scene, especially with its so obviously CGI'd skydive.
The Parkour chase in CR did have me experiencing a fear of heights in the theater though.
Another thought I've been having, and this is a good thread for it, is Craig's 'blunt instrument' of Bond constantly breaking through things (dry wall in CR's construction site, for example.) Whereas Connery/Lazenby/Brosnan's 007 finds out how to open a secret door, Craig just smashes through the wall to a secret room. Whereas Lazenby (or was it Tracy), ski jumps off snowy roofs of houses, Craig plows right through them with a plane, intentionally taking out two cars in the process. Whereas Dalton misses shooting his target through a window, Craig takes out three baddies and the bomb which then blows the entire building. "Bottoms up."
His vehicles are left doorless, wingless, landing gear-less, parked at the bottom of a river, rolled a world record number of times, Volkswagons crushed like beetles. Houses sunk, buildings exploded, hotels engulfed, and a Guinness World Record setting explosion in a crater. He's the unstoppable force.