Tony Award-winning director Daniel Sullivan ("Proof") will stage the production, which will see LaBeouf play a petty thief who kidnaps a rich older man (Baldwin). Complicating matters, LaBeouf's character looks after a damaged sibling, and the pair gradually form a parental bond with the man they've imprisoned.
Though the play was first performed in 1983 and has been a vehicle for everyone from Albert Finney to "Risky Business" star Joe Pantoliano, this will mark its first appearance on the Great White Way. A 1987 film version was made by Alan J. Pakula, but received mediocre notices.
Performances of the LaBeouf-led "Orphans" will begin on March 19, 2013, and the show will officially open on April 7, 2013, at the Schoenfeld Theatre.
Casting for the role of LaBeouf's brother will be announced later, producers said.
For LaBeouf, the role is a chance to demonstrate he's a real actor in addition to a movie star. Though he made a name for himself in blockbusters like "Transformers" and "Indiana Jones and the Kingdom of the Crystal Skull," he has been appearing in edgier fare like last summer's crime drama "Lawless" and Lars von Trier's upcoming sex opus "Nymphomaniac."
Other credits include "Holes" and "Wall Street 2: Money Never Sleeps."