The actress and humanitarian described the act as one of 'unthinkable cruelty' in a press conference to promote latest film Maleficent.
'Sadly, of course, there is real evil in the world. You watch the news and you see all of the people suffering so much cruelty' said the star.
Angelina's comments come a day after the leader of a Nigerian Islamic Group released a video taking responsibility for kidnapping the girls, also revealing plans to sell them on as slaves.
'They are slaves and I will sell them because I have the market to sell them'
'They are slaves and I will sell them because I have the market to sell them' said the leader of Boko Haram - which translates into 'Western education is sinful.'
He added: 'Girls, you should go and get married.'
Armed members of the group snatched the 276 girls from their beds in a remote part of Nigeria - forcing them into trucks and disappearing into the night. They were kidnapped because they were getting an education, something which the group believe girls and women have no right to.
Jolie, who is a Special Envoy of UN High Commissioner for Refugees, denounced the crime, and has lent her support to an online petition asking the Nigerian government to protect other girls at schools in the country.
Queen Latifah, Mia Farrow and Alyssa Milano have also spoken out about the situation, with the U.S. president sending a 'co-ordination cell' over the the African state to help locate the lost girls.