Jolie, a goodwill ambassador for the United Nations' refugee agency UNHCR who visited the Libyan-Tunisian border, said recent arrivals from Libya had told her about heavy fighting, harassment and assaults.
More than 400,000 people have fled Libya to Tunisia, Egypt, Niger, Algeria, Chad and Sudan since February when rebels rose up against Libyan leader Muammar Qaddafi. More than half have arrived in Tunisia.
"The international community has done well to reinforce Tunisia's remarkable relief effort," Jolie said in a UNHCR statement. "But with 2,000 people still crossing each day, we cannot let the funding dry up and need to sustain the momentum."
She also appealed for measures that would allow the U.N. and non-governmental organisations to access Libya and distribute urgent assistance, including food and medical supplies.
At the end of February, transit facilities were erected 7 km inside Tunisia to provide temporary shelter for those arriving from Libya and UNHCR and the International Organisation for Migration (IOM) organised humanitarian air evacuations.
More than 70,000 people have returned home with the help of UNHCR and IOM but more continue to arrive. Some 11,000 third country nationals are still in transit.
UNHCR said Jolie's family Jolie-Pitt foundation had covered the costs for a flight of 177 people and bought an ambulance to help support Tunisian efforts to assist the wounded.
There are some 2,500 people who are originally from war-torn countries and are unable to return home, UNHCR said.
"They're waiting here with little hope, unable to return home and unsure of what's to come. This constant cycle of displacement must finally come to an end," Jolie said.
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