The Hollywood superstar, who made her directorial debut in 2011 with Bosnian war drama In The Land Of Blood And Honey, is said to be in "final" talks to take control of Laura Hillenbrand's Unbroken: A World War II Story Of Survival, Resilience And Redemption, reported Deadline.
Angelina will reportedly "oversee" the fine-tuning of the script, which has been drafted by Les Miserables screenwriter William Nicholson.
The film - which tells the true story of former Olympian and WWII bombardier Louis Zamperini - has been in the works since Universal acquired the book rights in January 2011.
Francis Lawrence, who directed I Am Legend and Water For Elephants and is in charge of The Hunger Games sequel Catching Fire, had been attached to the director's role.
Production on Unbroken is expected to begin in 2013.
Angelina, who has six children with fiance Brad Pitt, is set to appear in front of the cameras again in Maleficent, which is due out in 2014.