The 35-year-old actress said she met with many people whose lives have been devastated by the floods, including mothers who lost their children and an elderly Pakistani couple who feared they would never be able to rebuild the home they lost.
"I am very moved by them and I hope that I am able to, today and tomorrow, be able to do something to help bring attention to the situation for all of the people in need in Pakistan," Jolie told reporters after visiting a refugee camp in the Jalozai area.
She toured the area wearing a long black robe and a black headscarf adorned with a thin red stripe -- the kind of conservative clothing worn by many Muslim women in Pakistan.
The floods began in the northwest at the end of July after extremely heavy monsoon rains and slowly surged south along the Indus River, swallowing up hundreds of villages and towns and killing more than 1,700 people. Another 17 million have been affected by the floods, and many will need emergency assistance to survive.
The United Nations issued an appeal for $460 million in emergency funds on Aug. 11, but only $294 million, or 64 percent, has been received so far, and donations have more or less dried up in recent days.
Ajay Chhibber, a U.N. assistant secretary general, said he hopes Jolie's visit will have "a very big impact" on the inflow of aid money and will keep people focused on the crisis.
"We need more ... well-known figures who can keep the spotlight and focus because people tend to forget internationally," said Chhibber, who is also the U.N. development agency's regional director for Asia. He spoke to reporters during a visit to Islamabad.