Steve Buscemi Enoch "Nucky" Thompson Actor Kelly Macdonald Margaret Schroeder Actor Michael Shannon Nelson Van Alden Actor Stephen Graham Al Capone Actor Vincent Piazza Lucky Luciano Actor Paul Sparks Mickey Doyle Actor Michael Kenneth Williams Chalky White Actor Gretchen Mol Gillian Actor Ben Rosenfield Willie Thompson Actor Jeffrey Wright Dr. Valentin Narcisse Actor Domenick Lombardozzi Ralph Capone Guest Star Marc Pickering Deputy Sheriff Enoch Thompson Guest Star Margot Bingham Daughter Maitland Guest Star John Ellison Conlee Commodore Louis Kaestner Guest Star Travis Tope Joe Harper Guest Star Paul Calderone Arquimedes Guest Star Louis Cancelmi Mike D'Angelo Guest Star Terence Winter Executive Producer Martin Scorsese Executive Producer Timothy Van Patten Executive Producer Stephen Levinson Executive Producer Mark Wahlberg Executive Producer