"The Boys & Girls Club exerted a profound influence on me and so many of my peers growing up, and I consider it an honor to give back," Washington said in a statement.
"I spent more than a decade as a member of the club in Mount Vernon, and I'm extremely pleased the production is willing to make 'American Gangster's' premiere a benefit for an organization that plays such an important, positive role in the lives of young people today."
Another Boys & Girls Club alumnus, Cuba Gooding, Jr., also stars in the film.
The premiere will be held on Oct. 19 at the Apollo Theater in Manhattan.
The film, which opens nationwide on Nov. 2, is based on the true story of criminal mastermind Frank Lucas who came up from the streets of 1970s Harlem.