Starring Frances McDormand in the title role, "Olive Kitteridge" is based on Pulitzer Prize-winning novel by Elizabeth Strout and follows a woman observing affairs, crime and tragedy in her small New England town.
Smith will play Kevin Coulson, an ex-student of Olive's, who returns to the small town. The cast also includes Richard Jenkins.
Smith was most recently seen in Breakfast at Tiffany's. His stage work also includes The Whale, Cock and The Shaggs: Philosophy of the World.
Tony and Oscar winner McDormand's stage credits include Awake and Sing!, A Streetcar Named Desire, The Country Girl and Good People. Her film work includes "Fargo," "North Country," "Burn After Reading," "The Man Who Wasn't There" and "Miss Pettigrew Lives for a Day."
Smith has also been cast in writer-director Peter Sattler's "Camp X-Ray." The film will feature Kristen Stewart as a young soldier assigned to Guantanamo, where Smith's character is also stationed.