And she's already taking the next steps to retiring from acting by getting plenty of buzz as a director, especially for her latest project Unbroken, which is based on the incredible life story of Olympic runner-turned-U.S. airman Louie Zamperini.
"I didn't ever think I could direct, but I hope I'm able to have a career at it because I'm much happier," she says about her new role behind the camera.
This isn't the first time Angelina has talked about quitting acting. In 2012, she told Britain's Channel 4 News that she would happily give up her career to be at home with her children.
"I am so grateful to the job, and I have had great experiences, and I have even be able to tell stories and be a part of stories that mattered and I have done things for fun, but ... if it went away tomorrow I would be very happy to be home with the children," she said. "I wake up in the morning as a mom and I turn on the news like everybody else, and I see what's happening and I want to be part of the world in a positive way."
Thankfully for her fans, that day isn't coming anytime soon.
Angelina is starring in the highly anticipated By the Sea with her husband Brad Pitt, a period love story which she wrote and is also directing. Her 13-year-old son Maddox is also working as a production assistant on the film.
Though predictably, it's not always easy working with your significant other.
"The tricky thing is directing myself and directing Brad," she admits. "It's hard, dramatic material, and we're balancing."
"It's a heavy film, and it's not easy for us," she adds. "But even as you struggle through it, you're in the trenches together and you don't expect it to be easy. We're challenging each other and that's a really good thing."
The last time Angelina and Brad starred in a film together was 2005's Mr. & Mrs. Smith. Now, nine years later, the two are married with six children.
"I think when it's right, it feels the exact same [as before]," she says about married life.