The Hollywood star and U.N. refugee agency's special envoy spoke as she visited the Zaatari camp, which hosts about 30,000 Syrians displaced by the 18-month conflict that has so far claimed at least 23,000 lives, according to activists.
"I am very concerned, the world is very concerned," Jolie said during her high-profile visit aimed at focusing international attention on the plight of Syrian refugees and attracting more funding to help them. "What is very heartbreaking is when Syrian people ask you why you think no one is able to find a solution for them."
"What they described on the ground, hearing it from them is so horrific," she said, adding that the children's stories were especially moving. "When you meet so many innocent people and civilians, the people of Syria are asking who is on their side. 'Who is going to help us as the months go on?''
The actress also said some of the refugees expressed fears "there will be no more of us" left in Syria as the relentless bloodshed grinds on.
Jolie also met separately with Syrian refugee women and toured the sprawling tent city in the company of U.N. refugee chief Antonio Guterres and Jordanian Foreign Minister Nasser Judeh.
"This mission that we are sharing has a key objective. It is to draw attention to the international community to express a much more stronger solidarity with Syrian refugees and the host countries that have kept their borders open to all those fleeing the conflict," said Guterres.
According to Guterres, Jordan has taken in some 200,000 Syrians - the largest number in the region. The refugee chief acknowledged the sheer numbers are taking a toll on Jordan's economy and resources, stressing that the "camp needs massive international funding" and that its conditions were "still not acceptable."
The UNHCR in April promoted Jolie from serving as its goodwill ambassador to special envoy due to her exceptional work for the agency.
Jordan opened up the Zaatari facility for Syrians in July after long delaying a decision on whether to set up refugee camps, possibly to avoid angering Syrian President Bashar Assad's autocratic regime by showing images at his doorstep of civilians fleeing his military onslaught.
Jolie was also to visit Syrian refuges in Lebanon, Turkey and Iraq during the rest of her trip to the region.
In Geneva, the UNHCR said Tuesday that while the agency has 253,106 people registered or awaiting registration as Syrian refugees, the real number is likely far higher since tens of thousands are believed to have not yet registered. Some are getting help from family or friends, while some are afraid to register for fear of possible consequences from Assad's regime.
Agency spokesman Adrian Edwards said the refugees have reported continuing artillery and air attacks in villages and towns close to the Jordanian border, and that there are thousands of displaced in southern Syria.
The UNHCR also has been scaling up emergency operations for 200,000 people inside Syria who have been displaced by fighting and need medical care, shelter and schools.