Dane DeHaan ("Chronicle") and Jack Huston ("The Twilight Saga: Eclipse") have also joined the cast of the film, directed and written by John Krokidas. He is a director of short films ("Slo-Mo," "Heroines"); this is first feature film.
"Kill Your Darlings" is based on the true story of the murder of David Kammerer that united Allen Ginsberg (Radcliffe), Kerouac and William Burroughs at Columbia University in 1944. Kammerer had been stalking Kerouac's friend, Lucien Carr (DeHaan), who became Ginsberg's love interest.
Olsen plays Edie Parker, a wealthy art student who was Kerouac's girlfriend and, eventually, his wife.
Principal photography for the movie starts March 12 in New York.
The movie is due to hit theaters in 2013.
Olsen, the younger sister of Mary-Kate and Ashley Olsen, made her big-screen debut in 2011 with leading roles in "Martha Marcy May Marlene" and "Peace, Love & Misunderstanding." She also stars in "Silent House," which hits theaters March 9.
Olsen is represented by The Gersh Agency. DeHaan is represented by CAA and The Schiff Company. Huston is represented by UTA.