The couple - who have been together for six years - have previously insisted they wouldn't tie the knot until gay marriage was legal throughout the US but the 'Moneyball' actor doesn't think they can "hold out" until then, particularly as their six children are keen to see them wed.
He said: "We made this declaration some time ago that we weren't going to do it till everyone can. But I don't think we'll be able to hold out.
"We'd actually like to, and it seems to mean more and more to our kids.
"It means so much to my kids, and they ask a lot. And it means something to me, too, to make that kind of commitment."
Brad and Angelina - who have biological kids Shiloh, five, and twins Knox and Vivienne, three, as well as adopted trio Maddox, 11, Pax, eight, and six-year-old Zahara - haven't ruled out adding to their brood further in future, with the actor appearing to suggest they are particularly keen to adopt again.
He added in an interview with The Hollywood Reporter: "We haven't closed the book on it.
"There's a really nice balance in the house right now, but if we see the need and get that lightning bolt that says 'We can help this person; we could do something here,' then absolutely."