The Only Girl (In The World) singer will take to the stage to help the Moneyball actor raise funds to build houses for people left homeless by Hurricane Katrina, according to The Hollywood Reporter.
The glitzy event in New Orleans in March - which will also promote the foundation's work to provide sustainable housing in other areas - will be hosted by Brad and US chat show host Ellen DeGeneres.
Other performers include Sheryl Crow and Seal, who recently split from his supermodel wife Heidi Klum.
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Sean Penn, Kevin Spacey, Spike Lee and Blake Lively will be among the A-list guests and comedian Aziz Ansari will host an after party.
Brad, who has six children with partner Angelina Jolie, created his Make It Right Foundation in 2007.