The Hollywood couple have pledged the staggering sum through their Jolie-Pitt Foundation to help refugees fleeing the Taliban in Pakistan.
Antonio Guterres, head of the United Nations Refugee Agency, has thanked Brad and Angelina for their generosity.
He said: "The situation in Pakistan is the most challenging humanitarian crisis of the past decade."
Earlier this week, Angelina - who has visited Pakistan three times in recent years - recorded a message highlighting the plight of displaced people living in war torn regions.
The 34-year-old actress - who is a Goodwill Ambassador for the United Nations High Commission on Refugees - says in the video: "Please don't turn away. Refugees are the most vulnerable people on Earth. Every day, they are fighting to survive. They deserve our respect. Please do not forget them. Remember them on this day. World Refugee Day."
World Refugee Day will be held on Saturday (20.06.09), but Angelina is to mark the day along with US Secretary of State Hillary Clinton in Washington today (18.06.09).
The donation comes just days after they gave $1 million to St. John's Hospital in Brad's hometown of Springfield, Missouri.
The money will be used to establish an endowment fund to pay for children's cancer specialists and will also go towards building a new paediatric unit.
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