Steve Buscemi Enoch "Nucky" Thompson Actor Kelly Macdonald Margaret Schroeder Actor Michael Shannon Nelson Van Alden Actor Shea Whigham Elias Thompson Actor Stephen Graham Al Capone Actor Vincent Piazza Lucky Luciano Actor Paul Sparks Mickey Doyle Actor Michael Kenneth Williams Chalky White Actor Jeffrey Wright Dr. Valentin Narcisse Actor Ben Rosenfield Willie Thompson Actor Gretchen Mol Gillian Actor Dominic Chianese Leander Whitlock Actor Arron Shiver Dean O'Banion Actor Stephen Root Gaston Means Actor Patricia Arquette Sally Wheet Guest Star Anatol Yusef Meyer Lansky Guest Star Ian Hart Ethan Thompson Guest Star Chris Caldovino Tonino Sandrelli Guest Star Giampiero Judica Salvatore Maranzano Guest Star Terence Winter Executive Producer Martin Scorsese Executive Producer Timothy Van Patten Executive Producer Stephen Levinson Executive Producer Mark Wahlberg Executive Producer