But now, the actress candidly admits to British Vogue that the past few years have been "really hard" for her and their six children, Maddox, 19, Pax, 17, Zahara, 16, Shiloh, 14, and 12-year-old twins Vivienne and Knox.
At one point in the interview, she is asked, "Do you feel as if you're at a happy stage in your life?" to which she responds, "I don't know."
"I've been focusing on healing our family," the Mr. & Mrs. Smith actress continues. "It's slowly coming back, like the ice melting and the blood returning to my body."
And though the 45 year old is unsure about her happiness at this time, she expresses excitement for her 50s, saying, "I feel that I'm gonna hit my stride in my 50s."
"Though we were on the trampoline the other day, and the children said, 'No, Mom, don't do that. You'll hurt yourself,'" she adds. "And I thought, 'God, isn't that funny?' There was a day I was an action star, and now the kids are telling me to get off the trampoline because I'll hurt myself."
But, as Angelina puts it, "I was never very good at sitting still."
She remarks that this desire for action and adventure has made motherhood slightly difficult, explaining, "I feel like I'm lacking in all the skills to be a traditional stay-at-home mom."
"Even though I wanted to have many children and be a mom, I always imagined it kind of like Jane Goodall, traveling in the middle of the jungle somewhere," Angelina continues. "I didn't imagine it in that true, traditional sense."
Nonetheless, the Oscar winner says she's "managing through it," thanks in part to her kids, who she described as "quite resilient."
"They're helping me, but I'm not good at it at all," she confesses.
The star previously shared that her kids have been her main priority, even revealing that she split from Pitt with them in mind.
"I separated for the wellbeing of my family," she said. "It was the right decision. I continue to focus on their healing."
And though reports have emerged about rifts between the kids and Brad, Angelina said their children know what really happened. She stated, "Some have taken advantage of my silence, and the children see lies about themselves in the media, but I remind them that they know their own truth and their own minds."
See the full feature in the March issue of British Vogue available via digital download and on newsstands Friday, Feb. 5.