Jolie, star of films such as "Mr & Mrs Smith" and also a UNHCR goodwill ambassador, spent two days meeting refugees, afterwards calling for more to be done to reintegrate former exiles into Afghan society.
Over 5.5 million people have returned to Afghanistan since 2002, the year after the Taliban were ousted by a US-led invasion, according to the UNHCR.
Most of them had fled to Pakistan and Iran and their return has increased the country's population by over 20 percent, it says.
There are currently some 140,000 international troops in Afghanistan fighting a Taliban-led insurgency.
"The focus needs to be put now on reintegration and that means not just putting up shelter but making sure there is water, job opportunities, a school for the children and medical clinics," Jolie said in a statement released by UNHCR at the end of the visit.
Jolie, married to fellow actor Brad Pitt, is noted for her humanitarian work. This was her second visit to Afghanistan, where she arrived Monday.
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