It was the couple's first official engagement since Jolie last week (ends13JAN06) announced to an aid worker that she is expecting the movie hunk's child.
The pair arrived on Haiti from neighbouring Dominican Republic, where Jolie is shooting THE GOOD SHEPHERD with Robert De Niro and Matt Damon, on Friday (13JAN06) and travelled in a convoy through the island's capital Port-au-Prince.
The couple then visited a school supported by FUGEES star Wyclef Jean's charity Yele Haiti.
Jolie told reporters, "You hear so much just about the danger and the fear, and then you come here and you meet just an amazing people.
"Given just a little chance, and given a little help, this is going to be a great country."
Meanwhile, Wyclef Jean has thanked his friends for taking the trouble to visit his homeland.
In a statement, the READY OR NOT hitmaker says: "To have these people grace our country is a beautiful thing."
Jolie and Pitt's visit to Haiti comes as the country struggles to organise its first elections since former President JEANBERTRAND ARISTIDE was forced from power during a violent coup in 2004.