Steve Buscemi (Nucky Thompson), Kelly MacDonald (Margaret Schroeder), Michael Shannon (Van Alden), Shea Whigham (Elias 'Eli' Thompson), Stephen Graham (Al Capone), Shae D'Lyn (Carolyn Rothstein), Byrne Davis Jr. (Whiskey Whiskers), Joe Fionda (agent FBI), Olivia Nikkanen (Fern), Vincent Piazza (Charles "Lucky" Luciano), Travis Tope (Joe Harper), Michael Kenneth Williams (Albert "Chalky" White), Paul Sparks (Mieczysław "Mickey" Doyle), Gretchen Mol (Gillian Darmody), Jeffrey Wright (Valentin Narcisse), Ben Rosenfield (William "Willie" Thompson), Dabney Coleman (Commodore Louis Kaestner), Michael K. Williams (Chalky White), Paz de la Huerta (Lucy Danziger), Michael Stuhlbarg (Arnold Rothstein), Aleksa Palladino (Angela Darmody), Michael Pitt (James 'Jimmy' Darmody)