"Next, we'll adopt," the actress says in an interview to air Tuesday on CNN's Anderson Cooper 360, the New York Post reports.
Jolie's two other children, 4-year-old Maddox and 16-month-old Zahara, were adopted from Cambodia and Ethiopia, respectively.
Her next child will be from another country, she says, although she hasn't decided which one or whether she's hoping to adopt a boy or a girl. "It's going to be the balance of what would be the best for Mad and for Z right now," she tells Cooper.
Jolie, 31, and Pitt, 42, are back in the United States with their three children. Pitt is in the process of adopting Maddox and Zahara.
According to the Post, Jolie tells Cooper she's inspired by the people she helps in her role as UN Goodwill Ambassador.
"You think, 'Jesus, the things these people go through,' " she says. "I owe it to all of them to get myself together and stop whining about being tired and get there and get focused because, God, it's the least I can do with what they live with."