Angelina, 38, was accompanied to the region by British Foreign Secretary William Hague as part of their campaign to stop the use of sexual violence as a weapon of war.
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Dressed in black, with a scarf to cover her head, Angelina joined Mr Hague to lay a wreath in front of a monument for the victims of the 1995 massacre. The pair then spoke to women who were raped during Bosnia's 1992-1995 war, as well as women whose loved ones were among the 8,000 Muslim men and boys killed in Srebrenica.
Earlier on Friday, Angelina and the British MP took part in a conference in the Bosnian capital of Sarajevo on sexual violence in war.
Angelina was accompanied by British Foreign Secretary William Hague during her visit to Bosnia
The actress, whose directorial debut In the Land of Blood and Honey dealt with violence against women during Bosnia's war, urged peace missions around the world to make combatting sex crimes a priority.
"The use of rape as a weapon of war is one of the most harrowing and savage of these crimes against civilians," she told the conference. "This is rape so brutal, with such extreme violence, that it is even hard to talk about it."
The pair laid a wreath at the monument for the victims of the 1995 Srebrenica massacre
Angelina, a goodwill ambassador for the UN for the refugee agency, and Mr Hague are due to co-host a high-profile summit on the same topic in London in June. Last March they visited a rescue camp for women in the Democratic Republic of Congo to highlight concerns over sexual violence.
Speaking of their visit to Bosnia, Mr Hague said, "Tens of thousands of women, girls and men were raped during the war in Bosnia. We are visiting to draw the world's attention to their search for justice, and to call for global action to end the use of rape as a weapon of war once and for all."
Earlier on Friday, the actress took part in a conference in the Bosnian capital on sexual violence in war
The pair hailed Bosnia's decision to include the prevention of sexual violence in military training as "ground-breaking".
Angelina said that the training was especially important for peacekeepers because their patrols "can mean that women no longer have to face a choice between going out for firewood and water and being raped, or seeing their children go hungry."