Jolie visited Syria in her role as a goodwill ambassador for the United Nations' refugee agency, UNHCR, and was accompanied by her partner, Brad Pitt, the agency said.
Tens of thousands of Iraqi refugees have returned home from Syria and other neighboring countries over the past year, but many more are unable or unwilling to return to a country still shaken by violence.
"Most Iraqi refugees cannot return to Iraq in view of the severe trauma they experienced there, the uncertainty linked to the coming Iraqi elections, the security issues and the lack of basic services," a UNHCR statement quoted Jolie as saying. "They will, therefore, be in need of continued support from the international community."
She was referring to Iraqi parliamentary elections scheduled for Jan. 16.
It was the Academy Award-winning actress' second visit to Syria in two years. On Friday, she visited Damascus' poorest suburbs where she was welcomed by two Iraqi families.
She also discussed the Iraqi refugee crisis with Syrian President Bashar Assad and his wife, Asma, UNHCR said.
UNHCR estimates that more than 4.2 million Iraqis have left their homes since the beginning of the conflict in 2003. To date, 215,000 Iraqi refugees are registered with UNHCR in Syria, the majority of whom are dependent on food and other material support.
The actress has worked with UNHCR since early 2001. In 2007, a foundation set up by Jolie and Pitt donated $1 million to help those affected by the conflict in Sudan's Darfur region and neighboring Chad.
Jolie has visited Iraq three times. Her last trip was in July, when she visited a settlement for displaced Iraqis in northwest Baghdad.