Her visit is part of her position as UN Special Envoy in which she speaks out on humanitarian issues.
Last year, she visited the UK to co-chair an event with Foreign Secretary William Hague on ending sexual violence in war zones.
The meeting took place after a screening at the Vatican of her film "Unbroken".
The Pope didn't watch it, but the actress along with two of her children met him briefly afterwards.
The 39-year-old star directed the film about American Olympian Louis (pron: louie) Zamperini, who survived in a raft after his plane was shot down during World War Two.
Angelina Jolie is said to have been raised as a Catholic but has recently talked about how she doesn't subscribe to any particular faith.
She said she would raise her children to be knowledgeable about them all so they can make up their own minds.