The Hollywood star arrived on Tuesday morning in the Zaatari camp, which hosts about 27,000 Syrians displaced by the 18-month conflict.
She met with Syrian refugee women separately and toured the sprawling tent city.
Jolie was accompanied by U.N. refugee chief Antonio Guterres and Jordanian Foreign Minister Nasser Judeh. Guterres said the "camp needs massive international funding" and that its "conditions are still not acceptable."
Jordan has sheltered more than 185,000 Syrian refugees - the largest number in the region.
The UNHCR in April promoted Jolie from serving as its goodwill ambassador to special envoy due to her work for the agency.
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