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.
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."
She said that efforts to aid refugees were "drastically underfunded" and that the system to deal with refugees was beginning to "break down."
This is "not because the model is flawed or because refugees are behaving differently, but because the number of conflicts and scale of displacements have grown so large," Jolie said, echoing recent comments made by U.N. agencies that the aid system is crumbling under the weight of conflicts.
Jolie's visit comes as Europe goes to extraordinary measures to deal with a massive influx of refugees, the biggest it has seen since World War II, with more than one million people crossing into the continent to seek asylum last year.
Several countries have erected razor-wire fences in what was once a much-celebrated post-war borderless zone as masses of refugees traverse Europe.
The European Union struck a deal with Turkey in which Ankara agreed to stop asylum-seekers from making the trip across the Aegean Sea. The EU has even started returning refugees who land in Greece, "swapping" them with others in Turkey who have been through an official registration process.
According to the United Nations, more than 180,000 refugees and migrants have tried to reach Europe by sea this year. More than 1,300 of whom have either lost their lives or been reported missing.
There are currently 60 million displaced people in the world, and of the 20 million refugees that made it out of their country last year, only 1 percent were resettled, U.N. figures show.