But they haven't ruled out adopting another child in the future.
Jolie, who is visiting earthquake victims in Haiti in her role as a UN Goodwill Ambassador, told CNN she was still open to expanding her "rainbow family".
She said: "I'm always open to children around the world. We're that kind of a family; Brad and I talk about that. But that's not what we're focusing on at this time, by any means.
"We're not here for that. We're here to see how we can help protect the children in country and scale up the needs here."
Pitt and Jolie already have three adopted children, Cambodian Maddox, eight, five-year-old Zahara, from Ethiopia, and Pax, six, from Vietnam.
They also have three biological children, Shiloh, three, and 19-month-old twins Knox and Vivienne.
The 34-year-old actress has also called for a restriction on adopting Haitian children in the aftermath of the earthquake.
"New adoptions should definitely not be encouraged as an immediate response to the emergency," she said.
"Haiti had many trafficking problems before the earthquake and now must keep a very close watch on the children. I would encourage as much support as possible to groups like UNICEF providing care for children in country."
The Telegraph reports that ten American missionaries are in jail in Haiti charged with child abduction and criminal conspiracy for trying to take 33 children across the border to an orphanage in the Dominican Republic.
Many of the chldren apparently still had parents, but some had handed over their children in the belief they could no longer care for them since the earthquake.