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The 29-year-old Pearl Harbour actor will take on the role of egotistical car salesman Charlie Babbitt (originally portrayed by Tom Cruise) in the play.
Brit actor Adam Godley (Son Of Rambow) has been cast as Babbitt's autistic brother Raymond, a role that won Dustin Hoffman an Oscar in 1989.
Hartnett said: "It has always been my intent to work on the London stage. It was only when I read the complex and charismatic character of Charlie Babbitt that I knew the time was right."
The stage version of Rain Man has been radically "re-imagined" for the present day. It will open at the Apollo Theatre in September under the direction of David Grindley.
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