According to CNN, when asked for her thoughts about Trump's attitude toward Muslims, Jolie closed her eyes and shook her head in disapproval.
"To me, America is built on people from around the world coming together for freedoms, especially freedom of religion. So it's hard to hear this is coming from someone who is pressing to be an American president," she said.
Trump's call to temporarily ban Muslims from entering the United States came as Syrians fled their war-torn homeland in the tens of thousands, with President Barack Obama pledging to take in 10,000 of them. CNN reports.
Jolie is just the latest figure to criticize Trump's remarks. Newly-elected London Mayor Sadiq Khan described them as "ignorant" and brushed off the candidate's fresher comments that he would make an exception for Khan and allow him to enter the country.
Jolie was speaking in London as the special envoy of the U.N. High Commissioner for Refugees at an event held by the BBC, where she made an impassioned plea for the world to unite in a coordinated response to the refugee crisis.
Jolie compared the situation to World War II, saying it was "that once-in-a-generation moment when nations have to pull together," warning against "fear of migration."