Yesterday she filmed being arrested by police, put in handcuffs and escorted out of a building.
She and the officers appeared to be covered in dust outside the courtyard of St. Bart's Church in Manhattan.
Two police officers escorted a dust-covered Angelina Jolie out of a New York building as part of a scene from her new movie Salt
The 33-year-old plays a CIA officer on a mission to clear her name after she is accused of being a Russian sleeper agent. She even gets to change her hair colour.
Her latest adventure comes just days after the 33-year-old filmed another equally action-packed scene.
Barefoot Angelina clings onto the wall - still with the nasty cut to her knee
She was again sporting a nasty cut to her knee - thought to be just make-up - which was visible during the scenes in Washington.
The Hollywood star's presence caused traffic to come to a standstill in the capital as she darted through vehicles and a crowd of extras, while cameramen could be seen hoisted on a cherry picker to get aerial shots.
Shards of glass can be seen showering down as Angelina clings on to the wall
After all the filming is done Angeline is helped in through a window, with a blanket to protect her knee from really getting cut
'I was surprised at how short she is,' worker Alexandra Kosmides told New Channel 8.
'If Angelina is here, Brad is here,' tourist Lindsay Galley added.
Stopping traffic: Angelina darts across the road, causing traffic to grind to a halt
'She's a character you never know,' the film's producer Lorenzo di Bonaventura said.
'People who think they know the real her may or may not. Those who think they can tell whether she's in a disguise also may or may not.
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'She tells you her agenda, but are you supposed to believe it?'
Stop: She hails down a taxi as a cameraman records the dramatic scenes
Husband Brad Pitt has accompanied his wife on the trip to Washington and was seen out with daughters Shiloh, two, and Zahara, four, over the weekend.
The Hollywood couple are reported to have called Zimbabwe's Premier Morgan Tsvangirai to offer condolences over his wife Susan's death in a car crash last week, it emerged today.
Get in: Angelina, sporting a blonde wig, plays the role of CIA officer Evelyn A Salt, who is accused of being a Russian spy
The couple are active in charity work around the world, but have no apparent links to Zimbabwe in particular.
Jolie gave birth to one of their children in nearby Namibia and the couple have adopted Ethiopian-born Zahara, among their six children.
Getting the best view: Cameramen are hoisted on to a cherry picker to record aerial shots on set yesterday
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