SOS Children's Villages is a global agency that says it focuses on family-based, long-term care of children.
Jolie is a United Nations goodwill ambassador.
SOS said the film star visited with and brought toys for the children, and met with President Rene Preval, current and former Haitian ministers, judges and lawyers, and U.S. State Department officials regarding child protection in the Caribbean island nation.
Before the overnight stay, Jolie held a dinner and roundtable discussion aimed at studying the Haitian legal system as it pertains to child protection issues and exploring mechanisms for strengthening the government's capacity to address these needs.
This is Jolie's second visit to an SOS facility in Haiti.
"I like to visit and support the SOS Children's Villages in the world because I have seen that the children are growing up in a safe and loving environment," Jolie said in a statement.
"Ms. Jolie's involvement helps to raise spirits when life has become so hard for children who have lost everything. Her continued support sheds an important light on the progress and challenges all of us face in Haiti," added SOS Children's Villages USA Chief Executive Officer Heather Paul. "With the 6-month anniversary of the earthquake approaching, Jolie helps the world remember that the struggle for survival continues on the ground every day. International partners working hand-in-hand with Haitians will be there for many years to come, long after the cameras have gone away."