Jane's Journey, a cinematic biography about Goodall, 77, chronicles her worldwide travels, personal footage from her childhood, and her charity work with Jolie.
"I was delighted when she told me she would be excited to be a part of the film," Goodall tells PEOPLE of Jolie, who meets with Goodall in the film inside her home to work on a sustainability project. "Sometimes, caught up in the moment, people promise to give their support but don't, or can't come through. That was not true with Angelina."
On Sept. 27, Jane's Journey will make its national debut in select theaters, along with a special live appearance by Goodall herself, in which she'll answers viewer questions.
The event will also features appearances by other famous friends of Goodall, including Pierce Brosnan and Dave Matthews.