Jolie heaped praise on Tunisia for the way it has been handling the problem after meeting with the Tunisian foreign minister, ending a two-day visit on Wednesday.
State news agency TAP quoted Jolie as offering the country her "solidarity."
Jolie visited the Tunisia-Libya border area on Tuesday.
The UNHCR says more than 400,000 people have fled from Libya over the last month amid fighting between rebels and longtime leader Moammar Gadhafi's forces.
The Associated Press contributed to this report.