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So this is yet another one of those split-second scenes.
Even if you don’t remember it, it’s a picture of Captain crappily roundhousing Loki, which I believe is still awesome.
What this scene probably looked like from the front
You know she knew that she had him. Of course, one could make the argument that Loki wanted to Natasha to “find out” about his plan with the Hulk, but that’s a whole theory in and of itself.