| Robert Stack | ... | Eliot Ness (118 episodes, 1959-1963) |
 | Walter Winchell | ... | Narrator (118 episodes, 1959-1963) |
| Nicholas Georgiade | ... | Agent Enrico Rossi / ... (86 episodes, 1959-1963) |
| Abel Fernandez | ... | Agent William Youngfellow / ... (69 episodes, 1959-1962) |
| Paul Picerni | ... | Agent Lee Hobson / ... (64 episodes, 1960-1963) |
| Steve London | ... | Agent Jack Rossman / ... (56 episodes, 1959-1963) |
| Bruce Gordon | ... | Frank Nitti (25 episodes, 1959-1963) |
| Jerry Paris | ... | Agent Martin Flaherty (16 episodes, 1959-1960) |
| Frank Wilcox | ... | Beecher Asbury / ... (13 episodes, 1959-1962) |
| Robert Bice | ... | Capt. Jim Johnson / ... (13 episodes, 1961-1963) |
| Anthony George | ... | Agent Cam Allison (12 episodes, 1960) |
| Oscar Beregi Jr. | ... | Joe Kulak / ... (8 episodes, 1960-1962) |
| Jason Wingreen | ... | Capt. Dorset / ... (8 episodes, 1960-1963) |
| Frank DeKova | ... | Anthony 'Tough Tony' Lamberto / ... (7 episodes, 1960-1962) |
| Grant Richards | ... | Arnie Retzik / ... (7 episodes, 1961-1963) |
| Barry Russo | ... | Brikka / ... (7 episodes, 1959-1962) |
| Chuck Hicks | ... | LaMarr Kane (6 episodes, 1959) |
| Harold J. Stone | ... | 'Tough' Tommy Karpeles / ... (6 episodes, 1960-1963) |
| Nehemiah Persoff | ... | Jake Guzik / ... (6 episodes, 1959-1962) |
| Herman Rudin | ... | Benny Rivas / ... (6 episodes, 1959-1963) |
| Joe De Santis | ... | Louis Latito / ... (6 episodes, 1959-1963) |
| Joseph Ruskin | ... | Louis 'Lepke' Buchalter / ... (6 episodes, 1959-1963) |
| Richard Reeves | ... | 1st Trucker / ... (6 episodes, 1959-1963) |
| Richard Bakalyan | ... | Benno / ... (6 episodes, 1960-1963) |
| K.L. Smith | ... | 'Puffy' Ocell / ... (6 episodes, 1960-1963) |
| Will Kuluva | ... | Frank Genna / ... (5 episodes, 1960-1963) |
| Gavin MacLeod | ... | Three-Fingered Jack White / ... (5 episodes, 1959-1962) |
| Michael Constantine | ... | Edmund Wald / ... (5 episodes, 1961-1963) |
| Phillip Pine | ... | Griff 'Ace' Darden / ... (5 episodes, 1959-1963) |
| Johnny Seven | ... | Canello / ... (5 episodes, 1959-1963) |
| Robert Carricart | ... | Charles 'Lucky' Luciano / ... (5 episodes, 1959-1963) |
| Bernard Fein | ... | Ed Harker / ... (5 episodes, 1960-1962) |
| Theodore Marcuse | ... | Alex / ... (5 episodes, 1960-1963) |
| Stewart Bradley | ... | Iggy Minter / ... (5 episodes, 1961-1963) |
| Joe Turkel | ... | Birdie Yates / ... (5 episodes, 1960-1963) |
| Cyril Delevanti | ... | Flophouse Manager / ... (5 episodes, 1960-1962) |
| Robert Middleton | ... | Mayor Anton J. Cermak / ... (4 episodes, 1960-1961) |
| Richard Karlan | ... | Danny Kurtz / ... (4 episodes, 1959-1961) |
| Ned Glass | ... | Art Rele / ... (4 episodes, 1960-1962) |
| Jay Adler | ... | Georgie Kaufman / ... (4 episodes, 1959-1962) |
| George N. Neise | ... | Archie Devlin / ... (4 episodes, 1960-1961) |
| Eugene Iglesias | ... | Emilio / ... (4 episodes, 1959-1962) |
| Vic Perrin | ... | Arnie Falken / ... (4 episodes, 1960-1963) |
| Penny Santon | ... | Emily Brodowski / ... (4 episodes, 1960-1963) |
| Byron Morrow | ... | Hartley Lester / ... (4 episodes, 1961) |
| Charles McGraw | ... | Barney 'Bugs' Birch / ... (4 episodes, 1959-1963) |
| Murray Hamilton | ... | Charley Mailer / ... (4 episodes, 1960-1962) |
| Milton Selzer | ... | Allan Sitkin / ... (4 episodes, 1961-1962) |
| Telly Savalas | ... | Leo Stazak / ... (4 episodes, 1960-1963) |
| Carl Milletaire | ... | Pete Konitz / ... (4 episodes, 1960-1962) |
| Antony Carbone | ... | Angelo Genna / ... (4 episodes, 1960-1963) |
| Wolfe Barzell | ... | Jake Brodowski / ... (4 episodes, 1960-1963) |
| John Harmon | ... | Arno Schwager / ... (4 episodes, 1959-1961) |
| Allen Jaffe | ... | Albert Cicciano / ... (4 episodes, 1959-1961) |
| John McLiam | ... | Driver / ... (4 episodes, 1961-1962) |
| Gene Roth | ... | Louis / ... (4 episodes, 1960-1963) |
| Dan Seymour | ... | Cy Brenner / ... (4 episodes, 1960-1962) |
| Don Gordon | ... | Frankie Gruder / ... (4 episodes, 1961-1963) |
| Bing Russell | ... | Cavanaugh / ... (4 episodes, 1960-1962) |
| Hugh Sanders | ... | Dr. Hasker / ... (4 episodes, 1959-1962) |
| Kenner G. Kemp | ... | Congressman Kerry / ... (4 episodes, 1959-1961) |
| Edward Asner | ... | Frank / ... (4 episodes, 1962-1963) |
| Frank Sutton | ... | Angie Stazak / ... (4 episodes, 1962-1963) |
| Jack Warden | ... | Frank Barber / ... (3 episodes, 1959-1960) |
| Luther Adler | ... | Charlie Zenko / ... (3 episodes, 1960-1962) |
| Norma Crane | ... | Alice Diamond / ... (3 episodes, 1960-1961) |
| Mike Kellin | ... | Abe Garfinkel / ... (3 episodes, 1960-1961) |
| Lawrence Dobkin | ... | Dutch Schultz / ... (3 episodes, 1959-1960) |
| Vaughn Taylor | ... | Dr. William A. Voyt / ... (3 episodes, 1959-1961) |
| Richard Carlyle | ... | Everett Lafferty / ... (3 episodes, 1959-1961) |
| Eddie Firestone | ... | Bitsy Whyller / ... (3 episodes, 1961-1963) |
| Lewis Charles | ... | Joe Giambatista / ... (3 episodes, 1960-1961) |
| Russ Conway | ... | Warden Hubbard / ... (3 episodes, 1961) |
| Arthur Kendall | ... | Machine Gun Machen / ... (3 episodes, 1960-1961) |
| Marc Lawrence | ... | Lou Cagan / ... (3 episodes, 1960-1963) |
| Harry Guardino | ... | Frank Odine / ... (3 episodes, 1960-1962) |
| Henry Silva | ... | 'Little' Charlie Sebastino / ... (3 episodes, 1960-1962) |
| Jack Elam | ... | Jug Alverson / ... (3 episodes, 1960-1962) |
| Robert J. Wilke | ... | Bugs Moran / ... (3 episodes, 1961-1962) |
| Steven Geray | ... | Eric Vajda / ... (3 episodes, 1960-1963) |
| Robert Ellenstein | ... | Felix Burke / ... (3 episodes, 1959-1963) |
| Linda Watkins | ... | Ada Spencer / ... (3 episodes, 1960-1963) |
| Phyllis Coates | ... | Angela Carney / ... (3 episodes, 1959-1962) |
| Harry Dean Stanton | ... | Moxie / ... (3 episodes, 1960-1961) |
| Dabbs Greer | ... | Agent Ned Ferber / ... (3 episodes, 1961-1963) |
| Steve Gravers | ... | Birch Henchman / ... (3 episodes, 1959-1963) |
| Frank Puglia | ... | Carlo Feruzzi / ... (3 episodes, 1959-1961) |
| Norman Alden | ... | Barry Carlton / ... (3 episodes, 1959-1960) |
| Raymond Bailey | ... | John Carvell (3 episodes, 1960) |
| Ben Wright | ... | Jacques Villon / ... (3 episodes, 1961) |
| A.G. Vitanza | ... | Cooker / ... (3 episodes, 1960-1962) |
| Sam Gilman | ... | Charlie Sherman / ... (3 episodes, 1960) |
| Paul Genge | ... | Deputy Police Chief Artie Bryson / ... (3 episodes, 1961-1962) |
| Lee Marvin | ... | Howard Carson / ... (3 episodes, 1961-1962) |
| Al Ruscio | ... | Denny Cole / ... (3 episodes, 1959-1963) |
| Simon Oakland | ... | Joe Palakopolous / ... (3 episodes, 1962-1963) |
| Claude Akins | ... | Jake 'Dodo' Ryan / ... (3 episodes, 1960-1963) |
| Robert Emhardt | ... | Fred Stegler / ... (3 episodes, 1960-1963) |
| Ed Nelson | ... | Johnny Prebble / ... (3 episodes, 1961-1963) |
| Paul Birch | ... | 'The King' Frank Argos / ... (3 episodes, 1961-1963) |
| Gilbert Green | ... | Henry Bogar / ... (3 episodes, 1961-1963) |
| Sheldon Allman | ... | Harry Mastrogeorge / ... (3 episodes, 1961-1963) |
| Jon Lormer | ... | Clary / ... (3 episodes, 1961-1962) |
| John Anderson | ... | George McPhail / ... (3 episodes, 1960-1963) |
| Baynes Barron | ... | Larry Rand / ... (3 episodes, 1961-1962) |
| Paul Dubov | ... | Charlie Banion / ... (3 episodes, 1961-1962) |
| Paul Bryar | ... | Police Capt. Reardon / ... (3 episodes, 1960-1962) |
| Tommy Nello | ... | Manny / ... (3 episodes, 1961-1962) |
| Hank Patterson | ... | Charlie--Warehouse Manager / ... (3 episodes, 1960-1962) |
| Olan Soule | ... | Dr. Amos Hallet / ... (3 episodes, 1960-1962) |
| Cliff Carnell | ... | Dolph Cagle / ... (3 episodes, 1962-1963) |
| Booth Colman | ... | Mike Pavanos / ... (3 episodes, 1962-1963) |
| Bill Erwin | ... | Auctioneer / ... (3 episodes, 1962-1963) |
| Jerry Oddo | ... | Fred Santos / ... (3 episodes, 1962-1963) |
| Malachi Throne | ... | Barnett / ... (3 episodes, 1962-1963) |
| John Kellogg | ... | Lucky / ... (3 episodes, 1962) |
| Martin Landau | ... | Jerry Fanning / ... (2 episodes, 1959-1961) |
| David Brian | ... | Brian O'Malley / ... (2 episodes, 1960-1961) |
| Steve Cochran | ... | Eddie Fletcher / ... (2 episodes, 1960-1961) |
| Joseph Wiseman | ... | Albert Maris aka Arnie 'The Wolf' Mendoza / ... (2 episodes, 1960-1961) |
| Neville Brand | ... | Al Capone (2 episodes, 1961) |
| Virginia Vincent | ... | Louise O'Hara / ... (2 episodes, 1959-1960) |
| Michael Ansara | ... | Charlie Steuben / ... (2 episodes, 1960-1961) |
| Larry Gates | ... | Carl D. Arnold / ... (2 episodes, 1960) |
| Joe Mantell | ... | Giuseppe 'Joe' Zangara (2 episodes, 1960) |
| Robert F. Simon | ... | Attorney General Homer S. Cummings / ... (2 episodes, 1960-1961) |
| Madlyn Rhue | ... | Chickie Bernstein / ... (2 episodes, 1960) |
| Peter Falk | ... | Duke Mullen / ... (2 episodes, 1960-1961) |
| Leo Gordon | ... | Pops Gantry / ... (2 episodes, 1960) |
| John Beradino | ... | Angie Viale / ... (2 episodes, 1959-1960) |
| David White | ... | Archie Grayson / ... (2 episodes, 1959-1960) |
| Betty Garde | ... | Alice / ... (2 episodes, 1959-1960) |
| Suzanne Storrs | ... | Dawn Dolan / ... (2 episodes, 1959-1960) |
| Peter Whitney | ... | 'Big' Bill Swinney / ... (2 episodes, 1960-1963) |
| John Marley | ... | Ed Carlton / ... (2 episodes, 1960-1961) |
| Ernest Sarracino | ... | Tomaso Fellini / ... (2 episodes, 1959-1960) |
| Arlene Martel | ... | Carla Patrone / ... (2 episodes, 1960-1961) |
| Val Avery | ... | Frank Salinas / ... (2 episodes, 1960) |
| Mort Mills | ... | Lulu Rosenkrantz / ... (2 episodes, 1959-1962) |
| Harry Bartell | ... | Dr. Olsen / ... (2 episodes, 1959-1961) |
| Meg Wyllie | ... | Mary O'Gara / ... (2 episodes, 1959-1962) |
| Peter Mamakos | ... | Gus Raddi / ... (2 episodes, 1959-1961) |
| Adrienne Marden | ... | Mrs. McGonigle / ... (2 episodes, 1960-1961) |
| Lalo Rios | ... | Tony Diaz (2 episodes, 1961) |
| Lee Van Cleef | ... | Frank Diamond (2 episodes, 1960) |
| Peter Baldwin | ... | Arthur 'Doc' Barker / ... (2 episodes, 1959) |
| Bernard Kates | ... | Davie / ... (2 episodes, 1960-1961) |
| Mario Gallo | ... | Chester / ... (2 episodes, 1961) |
| Vladimir Sokoloff | ... | Sam / ... (2 episodes, 1960-1961) |
| Howard Caine | ... | Blinky / ... (2 episodes, 1961) |
| Harry Shannon | ... | Joe Patterson / ... (2 episodes, 1959-1961) |
| John Wengraf | ... | Gus Kleeber / ... (2 episodes, 1960-1961) |
| James Flavin | ... | Rocky Garver / ... (2 episodes, 1960) |
| Percy Helton | ... | Jocko Monaghan / ... (2 episodes, 1960) |
| Joseph Mell | ... | Herschel Levitan / ... (2 episodes, 1959-1960) |
| Robert Cornthwaite | ... | Inspector Jim Goodrich / ... (2 episodes, 1961) |
| Lorna Thayer | ... | Connie LaVerne / ... (2 episodes, 1961) |
| Frank London | ... | Benny Marcus / ... (2 episodes, 1960-1961) |
| Francis De Sales | ... | Capt. Troy / ... (2 episodes, 1960) |
| Argentina Brunetti | ... | Angelo Cestari / ... (2 episodes, 1959-1960) |
| Vincent Barbi | ... | Big Augie Epstein / ... (2 episodes, 1960) |
| Paul Bruce | ... | Levine (2 episodes, 1961) |
| Ted Berger | ... | Moxie Harris / ... (2 episodes, 1960) |
| Alexander Lockwood | ... | Dr. Burley / ... (2 episodes, 1961) |
| John Daheim | ... | Rocky Pearson / ... (2 episodes, 1960-1961) |
| Jay C. Flippen | ... | Al Morrisey / ... (2 episodes, 1959-1962) |
| Steven Hill | ... | Jack 'Legs' Diamond / ... (2 episodes, 1960-1962) |
| Paul Richards | ... | Lou Sultan / ... (2 episodes, 1961-1963) |
| Rip Torn | ... | Harry Straus / ... (2 episodes, 1961-1963) |
| Victor Buono | ... | Melanthos Moon / ... (2 episodes, 1961-1962) |
| Richard Conte | ... | Arnie Seeger / ... (2 episodes, 1961-1962) |
| Cloris Leachman | ... | Julie Liemer / ... (2 episodes, 1961-1962) |
| J.D. Cannon | ... | Al Remp / ... (2 episodes, 1962-1963) |
| Sean McClory | ... | Captain John Stanwood / ... (2 episodes, 1962) |
| Darryl Hickman | ... | Danny Madikoff / ... (2 episodes, 1959-1962) |
| Christopher Dark | ... | Arno Beale / ... (2 episodes, 1960-1963) |
| John Hoyt | ... | Capone's Lawyer / ... (2 episodes, 1960) |
| John Larch | ... | Bryan 'Bull' Hanlon / ... (2 episodes, 1961-1962) |
| Collin Wilcox Paxton | ... | Ann Gratzner / ... (2 episodes, 1962) |
| Adam Williams | ... | Lloyd Barker / ... (2 episodes, 1959-1963) |
| Gail Kobe | ... | Rita / ... (2 episodes, 1960-1963) |
| Nita Talbot | ... | Alice / ... (2 episodes, 1960-1962) |
| Barry Morse | ... | Larry Bass / ... (2 episodes, 1961-1963) |
| George Voskovec | ... | Charles Tarasovich / ... (2 episodes, 1961-1963) |
| Martin Balsam | ... | Arnold Justin / ... (2 episodes, 1961-1962) |
| Kevin Hagen | ... | Jan Tobek / ... (2 episodes, 1961-1962) |
| Carroll O'Connor | ... | Arnie Kurtz aka Albert Krim / ... (2 episodes, 1961-1962) |
| Karl Swenson | ... | Hans Dreiser / ... (2 episodes, 1961-1962) |
| Salome Jens | ... | Eva Tobek / ... (2 episodes, 1962-1963) |
| Joe Di Reda | ... | Fred Barker / ... (2 episodes, 1959-1962) |
| Eduardo Ciannelli | ... | Gregory Pindar / ... (2 episodes, 1960-1962) |
| Jack Klugman | ... | Morton Halas / ... (2 episodes, 1961-1963) |
| Ted de Corsia | ... | Big Jim Harrington / ... (2 episodes, 1959-1962) |
| Ellen Madison | ... | Millie Joplin / ... (2 episodes, 1961-1962) |
| Virginia Christine | ... | Dora Mizo / ... (2 episodes, 1960-1963) |
| H.M. Wynant | ... | Boley Davis / ... (2 episodes, 1959-1963) |
| George Keymas | ... | Carl Dancing / ... (2 episodes, 1961-1963) |
| Alan Baxter | ... | Harry Mailer / ... (2 episodes, 1961-1962) |
| Stanley Adams | ... | Max Posen / ... (2 episodes, 1959-1963) |
| Ken Lynch | ... | Theodore 'Ted' Newberry / ... (2 episodes, 1959-1962) |
| Mike Mazurki | ... | 'Moose' Tobin / ... (2 episodes, 1959-1962) |
| Jeremy Slate | ... | Elroy Daldran / ... (2 episodes, 1960-1963) |
| Craig Duncan | ... | Gordo / ... (2 episodes, 1961-1962) |
| Paul Langton | ... | Bob Wheaton / ... (2 episodes, 1960-1962) |
| Bartlett Robinson | ... | Federal Judge James H. Wilkerson / ... (2 episodes, 1960-1961) |
| Joseph Bernard | ... | Alvin Stryker / ... (2 episodes, 1961-1962) |
| John Mitchum | ... | Brewery employee / ... (2 episodes, 1961-1962) |
| Paul Marin | ... | Sam Deroy / ... (2 episodes, 1962-1963) |
| Than Wyenn | ... | Leblanc / ... (2 episodes, 1962-1963) |
| Barbara Luna | ... | Lucita / ... (2 episodes, 1959-1962) |
| Frank Gerstle | ... | Police Captain / ... (2 episodes, 1959-1960) |
| Addison Richards | ... | Mayor Roy B. Gautier / ... (2 episodes, 1960-1961) |
| Robert Stevenson | ... | Jake Logan / ... (2 episodes, 1960) |
| Larry Breitman | ... | Chestnut Vendor / ... (2 episodes, 1961-1962) |
| Norman Burton | ... | Solly / ... (2 episodes, 1961-1962) |
| Michael Fox | ... | Bradley / ... (2 episodes, 1961-1962) |
| Barbara Pepper | ... | Lodger / ... (2 episodes, 1961-1962) |
| Toni Tucci | ... | Alma / ... (2 episodes, 1961-1962) |
| Michael Hinn | ... | Jethroe / ... (2 episodes, 1962-1963) |
| Alan Dexter | ... | Feeney / ... (2 episodes, 1960-1963) |
| Russ Bender | ... | Daniel Gosden / ... (2 episodes, 1961-1962) |
| Arny Freeman | ... | Webster / ... (2 episodes, 1961-1962) |
| Joseph V. Perry | ... | Cully Grice / ... (2 episodes, 1961-1962) |
| Tom Reese | ... | Georgie Summers / ... (2 episodes, 1960-1963) |
| Jack Reitzen | ... | Fat Mike / ... (2 episodes, 1961-1963) |
| Robert Beecher | ... | Boomer (2 episodes, 1961-1962) |
| Barnaby Hale | ... | Ned Beemis / ... (2 episodes, 1961-1962) |
| Harry Swoger | ... | Battler / ... (2 episodes, 1961-1962) |
| Murvyn Vye | ... | Lou Hyndorf / ... (2 episodes, 1961-1962) |
| Robert Karnes | ... | Harvey Sloan / ... (2 episodes, 1960-1963) |
| John Zaccaro | ... | Andrews / ... (2 episodes, 1960-1962) |
| Walter Burke | ... | Herbie Snow / ... (2 episodes, 1961-1963) |
| Brook Byron | ... | Madame Amy / ... (2 episodes, 1961-1962) |
| Andrea Darvi | ... |
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