- Vito Scotti - Dante
- Jack Cassidy - Mr. Bob
- Robert Middleton - The Whip
- Murray Alper - Contact Man
- Joey Forman - Harry Hoo
- Ernest Borgnine - TV Viewer (uncredited)
- Frank De Vol - Carleton
- John Milford - Greco
- Lee Bergere - Richelieu
- Harold Gould - Hans Hunter
- John Myhers - Otto Hurrah
- Percy Helton - A.J. Pfister
- Jack DeLeon - Stroheim
- Arlene Golonka - Zelda
- Alice Ghostley - Veralenya Sarconyacov
- Gayle Hunnicutt - Octavia
- Leonard Strong - The Claw
- Ellen Corby - Agnes Davenport
- Bob Hope - Room Service Attendant (uncredited)
- Victor French - Agent 44
- H.M. Wynant - Melnick Archer
- Gordon Jump - Hobson
- Elisa Ingram - Rena
- Don Rickles - Sid Krimm
- Victor Sen Yung - Abe Fu Yung
- Milton Selzer - Parker
- Nicholas Georgiade - Marcus
- Joseph Sirola - Harvey Satan
- Robert Easton - Maestro
- Kitty Kelly - The Woman / Mrs. Green
- James Komack - Gunman
- Ann Prentiss - Nancy
- Michael Dunn - Mr. Big
- Janine Gray - Zelinka
- Charles Bateman - Chuck Cramer
- Sheila Leighton - Greta
- Gilbert Green - Kimmel (as Gil Green)
- Kelton Garwood - Garth
- Inger Stratton - Princess
- Bobby Somers - Spinoza
- Bill Saito - Toto
- Sarah Marshall - Nicola
- Harold J. Stone - Captain Groman
- Sid Haig - Bruce
- Sid Haig - Guard
- Sid Haig - Turk
- Lee Kolima - Bobo
- Jan Arvan - Sehokian
- Paul Lukather - Baccardo
- Viviane Ventura - Consuela Merendez
- Viviane Ventura - Consuela
- Nancy Kovack - Sonja
- John Harding - Marco
- Allen Emerson - Luchek
- Judy Lang - Mildred Spencer
- Alice Reinheart - Hilda
- Tim Herbert - Attendant
- Victoria Carroll - Myrna
- Barbara Stanek - Vana
- Jayne Massey - Nina
- Rose Michtom - Customer at Richelieu's (uncredited)
- Rose Michtom - Woman at the Pool (uncredited)
- Ann Elder - Dr. Simon
- Nancy Walters - Dr. Hans Svenson
- Bernie Kopell - Siegfried
- John Sebastian - KAOS Agent #2
- Diahn Williams - Bohrman
- Diahn Williams - Van Cleef
- Warde Donovan - Hotel Doctor (as Ward Donovan)
- Dick Cherney - Party Guest (uncredited)
- Dick Cherney - Man at Pool (uncredited)
- Al Bain - Marathon Spectator (uncredited)
- Martin Ashe - Agent 42
- Ted de Corsia - Spinoza
- Pat O'Hara - Judge
- Jim Boles - Dr. Ratton
- Anthony Larry Paul - KAOS Agent at Airport (uncredited)
- Anthony Larry Paul - Ravage
- Ward Wood - Busby
- Karen Norris - Mother
- David Ketchum - Agent 13
- Richard Gautier - Hymie
- Hal Taggart - Party Guest (uncredited)
- Conrad Janis - Victor
- Charles Lane - Uncle Abner
- Maudie Prickett - Aunt Bertha
- Maudie Prickett - Naomi Hickenlooper
- Victor Buono - Hannibal Day
- Leo Gordon - Grillak
- Larry Storch - Groovy Guru
- Henry Brandon - Zukor
- Henry Brandon - Belasco
- Barry Newman - Assistant Guru
- Peter Brocco - Professor Pheasant
- Phyllis Diller - Maxwell Smart (uncredited)
- Martin Landau - Maxwell Smart (uncredited)
- Woodrow Parfrey - Dr. Pasteur
- Sharon Acker - Dr. Simon (uncredited)
- Jack Perkins - Gregor
- Len Lesser - Luden
- Len Lesser - Vogel
- Len Lesser - Rudolph
- John McLiam - Seidlitz
- Norman Burton - Control Agent (uncredited)
- Ina Balin - Ann Ferris
- Michael Forest - Basil
- John Doucette - Colonel Von Klaus
- Johnny Carson - Herald (uncredited)
- James Caan - Rupert of Rathskeller (uncredited)
- Eddie Hice - KAOS Agent (uncredited)
- John Dennis - Kinsky
- John Fiedler - Felix
- John Fiedler - Mr. Hercules
- Joseph Mell - Preminger
- Joseph Mell - Waiter
- Nick Dimitri - Nightclub Patron (uncredited)
- Byron Foulger - Bush
- Burt Mustin - Agent #8
- Ted Gehring - Mace
- Gary Nelson
- Jay Sandrich
- Burt Nodella
- Chris Hayward
- Jess Oppenheimer
- James Komack
James Caan interpreta a Rupert of Rathskeller (uncredited) en la serie.
Ted de Corsia interpreta a Spinoza en la serie.
Martin Landau hace el papel de Maxwell Smart (uncredited).
Don Adams interpreta a Maxwell Smart en la serie.
Barbara Feldon interpreta a Agent 99 en la serie.
Edward Platt hace el papel de Thaddeus.
Robert Karvelas interpreta a Larabee en la serie.
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