The Hollywood couple gave the generous contribution to St. John's Hospital in the actor's hometown of Springfield, Missouri, over the weekend, reported contactmusic.com.
The treatment unit will be renamed the Jane Pitt Pediatric Cancer Center in honour of Pitt's mother who is very passionate about children's health issues.
The money will also go towards building a new paediatric unit, a 10-bedroom hospice and increasing the size of the neonatal and paediatric intensive care units.
Jolie and Pitt, who have three adopted and three biological children, last year donated over $8 million to charity.
--IANS