But the 38-year-old has opened up in a rare and candid interview, revealing that she thought she would never find love, or have children.
"I never thought I'd have children, I never thought I'd be in love, I never thought I'd meet the right person," Angelina tells Elle magazine, on whose cover she appears in June.
Angelina Jolie with her partner of nine years, Brad Pitt
The brunette beauty attributes this to coming from a broken home: "Having come from a broken home – you kind of accept that certain things feel like a fairy tale, and you just don't look for them."
Angelina, who has been with her partner Brad for nine years and engaged for two, and with whom she has six children, Maddox, Pax, Zahara, Shiloh and twins Vivienne and Knox, talks about the evolution of her relationship with 50-year-old Brad.
Angelina and Brad pictured arriving in Los Angeles with their brood
"You get together and you're two individuals and you feel inspired by each other, you challenge each other, you complement each other, drive each other beautifully crazy," she says.
"After all these years, we have history—and when you have history with somebody, you’re friends in such a very real, deep way that there’s such a comfort, and an ease, and a deep love that comes from having been through quite a lot together."
Angelina with young daughter Vivienne Jolie-Pitt
As well as talking about life and love now, the Maleficent star also opens up about her famous past behaviour, such as when she kissed her older brother James on the Oscars red carpet in 2000 and when she carried ex-husband Billy Bob Thornton's blood in a vial around her neck.
When you're young, Angelina says, "You want to be free. And as you start to feel that you are being corralled into a certain life, you kind of push against it. It may come out very strange, it may be interpreted wrong, but you're trying to find out who you are."