Cover Girl: Angelina Jolie on Marie Claire Magazine

Actress and activist Angelina Jolie is everywhere lately, busily promoting her newest film, A Mighty Heart. This month, she's on the cover of Marie Claire magazine, dishing about her life with Brad Pitt, their four kids and her charitable causes.

If a wild-child role in Girl, Interrupted seemed just the right outlet for Jolie in her 20s, a project like A Mighty Heart, about geopolitics and real love, seems perfect for her now. Along with her far-reaching humanitarian work, Jolie, 32, has a real love -- perhaps you've heard -- with Pitt, whom she met while making 2005's Mr. and Mrs. Smith. "I wasn't looking at the time," Jolie says. "I was quite happy having lovers and being a single mom" -- to Maddox, whom she'd adopted in March 2002 from a Cambodian orphanage with second husband Billy Bob Thornton. "The last thing I was looking for was somebody to have a relationship with."

Now it's Jolie and Pitt, together, visiting sites of deprivation around the globe -- touring earthquake-devastated Pakistan in 2005, spending Christmas with Colombian refugees in Costa Rica last December -- trying to marshal resources for desperate families as part of Jolie's work as the Goodwill Ambassador of the United Nations High Commission on Refugees; there is also the Jolie-Pitt Foundation, through which they donated $1 million in May to relief efforts in Darfur. Reflecting the degree to which the personal and the political are, for them, inextricable, they purchased a home at yet another site of unimaginable devastation, New Orleans, where Pitt has been laboring to put his love of green architecture and construction to good use. "It's a very big, very frustrating, complex problem," Jolie says. "I see Brad working so hard -- working out some building, mapping out a street -- and then we're sitting there, and another mother is talking about how the levees aren't fixed." She can't hide her annoyance. "Big decisions aren't [being] made on a higher level -- it is so much wasted effort. I have gotten really frustrated with the sense of a lack of justice in the world."

If Jolie and Pitt are united in their causes, they seem virtually fused in parenthood. In addition to Maddox, who's about to turn 6, there is 2-year-old Zahara, adopted from Ethiopia in 2005; 3-year-old Pax, whom Jolie brought home from Vietnam in 2007; and 14-month-old Shiloh, their biological daughter.

To read more from the "Angelina Unbound" cover story, check out the July issue of Marie Claire, on sale now!

Photo from Marie Claire.