According to Deadline, Brosnan will join lead Owen Wilson in the film, about an American who relocates his family to Southeast Asia and becomes entangled in a violent coup.
Brosnan will reportedly be playing a mysterious government spy in the action thriller, written by Devil director John Erick Dowdle and his brother Drew Dowdle.
Sources close to the film say that it will have the tone of Liam Neeson's 2008 hit Taken, marking a return for Wilson to the action genre.
Filming on The Coup is scheduled to begin this October.
Brosnan most recently starred opposite Sarah Jessica Parker in I Don't Know How She Does It.
He is also gearing up to star in the adaptation of the Nick Hornby novel A Long Way Down opposite Toni Collette.