The UN Goodwill Ambassador toured devastation sites in Misrata and Tripoli, where battles have raged between revolutionaries and forces loyal to former leader Moammar Gadhafi.
Jolie said she is inspired by the Libyan people's desire to fight for their rights after decades of oppression.
She explained to Reuters: "What's extraordinary... is that a lot of the people who are part of the solution and are working in positions of even military, and you find that just before the revolution they had retired, or were running restaurants or were selling baby clothes and they've all quit their jobs and they are all working here now on behalf of their country.
"They have all lost family members... they've suffered casualties themselves, they've lost limbs themselves and yet they're all really fighting for something they believe in, and for the future of the country for their children, so it's quite moving."
During her trip to Libya, Jolie met with members of the interim government and refugees who have fled their homes amid the bloodshed.
"I'm also here on behalf of the Libyan people to show them solidarity," she said. "I think this revolution on behalf of human rights, which is what I feel these people really have been doing and what they have pushed for, and to help them to implement these new laws and help them with the future of their country."
Sean Penn praised the Libyan people for showing "the courage to say [they] want freedom" during his own recent visit to the country.
Earlier this month, the UN paid tribute to Jolie's humanitarian efforts at a gala dinner in Switzerland.Source
