Jolie, a U.N. refugee agency goodwill ambassador, toured the outskirts of Kabul.
At one point, she toured a former warehouse that is now home to 50 families.
It is one of 30 informal settlements in Kabul where people struggle to survive in the cold winter months.
"It is clear traveling through the country, that what needs to be done is a very focused approach on these places of return, this idea of what return is and the difference between just returning and reintegrating," said Jolie.
Jolie later added her voice to calls by United Nations agencies to protect civilians displaced by conflict in Libya.