The actress, a Goodwill Ambassador for the United Nations refugee agency (UNHCR), has been travelling across the war torn and poverty-stricken region since September (09) and she was joined by Pitt as she continued her tour with a stop in Jordan.
The couple made a trip to the SOS Children's Village in Amman on 1 October (09) after accepting an invitation from American-born Queen Noor, who serves as the Honorary Chairman of the charity.
It was Jolie's second time in the village after previously promising to pay for the running costs of one family's home during a 2003 visit to Jordan.
And Jolie was delighted to see how well the village was being run.
She says, "The SOS model of providing care for children without parental care is one of the best, as they are still in a family setting within their own country.
"We hope more people learn about their programmes and give them support."
Jolie has also met with Somali refugees in Kenya, while Pitt accompanied her to meet with Iraqi refugees in Syria in recent weeks.