The couple are planning to adopt a child from a Syrian refugee camp and have one more biological child.
The couple famously share a brood of six, including adopted children from Cambodia, Vietnam and Ethiopia.
According to UK newspaper The Sun, the actress is eager to adopt once again.
She has apparently set her heart on taking in a little girl from Jordan after visiting Syrian refugees there earlier this month.
"She has been particularly touched by the situation in Syria and wants to adopt a child from Jordan to do her bit to help. The publicity would help draw the world's attention to what's going on there," a source said, adding, "They're crossing their fingers that they'll bring their next child home soon."
The couple also hope to have another biological child, according to the report.
Now that their youngest are thriving at age four, Brad and Angelina seem to feel it's the perfect time for more.
Apparently Angelina is preparing for a pregnancy already by making sure she's eating healthfully.
"Angie and Brad also want to have one more biological child so she is eating a diet rich in potassium," the source said.
Angelina, 38, revealed in May she underwent a double mastectomy after tests revealed she had a mutated gene which increased her risk of breast cancer.
Reports suggest she plans to go under the knife before turning 40 to remove her ovaries, which could also be affected.
She opened up about her medical decision in a New York Times op-ed piece. The actress stated her biggest motivators were her kids.
"I can tell my children that they don't need to fear they will lose me to breast cancer," she wrote.
Angelina adopted son Maddox from a Cambodian orphanage in 2002 when he was seven months. Daughter Zahara was six months when she adopted from Ethiopia in 2005 and son Pax was three when he was adopted from Vietnam two years later.
They welcomed their first biological child, Shiloh, in 2006, and then had twins Knox and Vivienne two years later.
The longtime couple are believed to be planning their wedding for this summer.
"Angie and Brad are even more into their family after her recent health scare. It has focused them on what's important in life," the source said.