The Hollywood celebrity and goodwill ambassador for the U.N. High Commissioner for Refugees arrived in the Turkish province of Hatay on a private jet with boxes of toys for the refugee camps.
She visited one of the three refugee camps in Turkey, where nearly 10,000 Syrian have sought refuge.
Jolie spent over two hours with about 1,700 refugees at a camp about 12 miles away from the Syrian border, sharing fruit and desert with them and speaking with them through an interpreter, Turkey's NTV television reported.
"The people in this camp have fled in fear for their lives, and many told me they were distraught about the safety of loved ones still in Syria." Jolie said in a UNHCR statement.
The actress praised Turkey for welcoming the refugees, saying it is critical in these situations that people have access to safety.
"I am really grateful for the open-door policy of Turkey in allowing these people to enter and the assurances that there will be no forced returns," she said.
Protests first erupted in Syria in mid-March as part of the "Arab Spring" push toward democracy. Syrian President Bashar Assad responded by unleashing the military to crush the street demonstrations. Human rights activists say more than 1,400 Syrians have been killed and 10,000 detained.
Jolie made a similar trip in April, traveling to Tunisia to meet with people who had fled war torn Libya.
The Associated Press contributed to this report.