- Richard Anderson - Senator Steve Bryant
- Alexander Scourby - Professor Amadeus / Wolfgang Wolp
- Joan Freeman - Clemency McGill
- Pat Crowley - Elaine May Donaldson
- Ivan Dixon - Jean Francis Soumarin
- Rupert Crosse - Nobuk
- Fritz Weaver - Andrew Vulcan
- Herbert Lom - Randolph
- Kim Darby - Sandy True
- Joan Crawford - Amanda True
- Curd Jürgens - Carl Von Kesser
- Telly Savalas - Count Valeriano De Fanzini
- Terry-Thomas - Constable
- Patricia Medina - Lucia Belmont
- Julie Sommars - Mimi Doolittle
- Vincent Price - Victor Marton
- Adam Roarke - Cantrell
- Dodie Marshall - Receptionist
- Sheila Leighton - Salesgirl
- Danica D'Hondt - Lucia Nazarone
- Sharon Tate - Therapist
- Susan Odin - Melissa Hargrove
- Charles McGraw - Jules Cutter
- Jay D. Jones - Prof. Walter Powers
- Valora Noland - Grand Duchess Vicky
- Linda Gaye Scott - Suzy
- Claude Akins - El Supremo
- Rodolfo Acosta - Captain Ramirez
- Ken Renard - Dr. Delgado
- Isabel Cooley - Conchita Delgado (as Isabelle Cooley)
- Maidie Norman - Mama Lou
- John Alvin - Doctor
- Ann Elder - Joanna Sweet
- Maurice Evans - Sir Norman Swickert
- Vera Miles - Madame Raine De Sala
- Bernard Fox - Jordin
- William Corcoran - Ronny (uncredited)
- William Corcoran - Sammy Sparks
- Charles Drake - Taggart Coleman
- Nobu McCarthy - Monica Hyodo
- Robert Ellenstein - Doctor Ieato
- Charles H. Radilak - Ambassador Vanderloon (as Charles H. Radilac)
- Eric Feldary - Kramer
- Jacqueline Dalya - Countess
- Karen Carlson - Helene
- Jay North - Bartlett Warshowsky
- Richard Peel - Cat Man
- Sid Haig - Alex
- Sid Haig - Vito
- Anthony Larry Paul - Commander Jenkins
- Diana Hyland - Miranda Bryant / Irina
- Anna-Lisa - Signe
- Carroll O'Connor - Walter B. Brach
- Joan O'Brien - Chris Brinel
- Shuji J. Nozawa - Chuke (as Shuji J. Nozawa)
- Neile Adams - Sita Chandi
- Juliet Mills - Eva
- Norbert Schiller - Little Man [Dr. Ingster]
- Sol Gorss - Konrad
- Ted de Corsia - Chief Highcloud
- Nicholas Colasanto - Ralph
- William Marshall - Premier Sekue Ashumen
- Victoria Shaw - Gracie Ladovan
- Robert Brubaker - Assassin
- Martin Landau - Count Ladislaus Zark
- Jack Palance - Louis Strago
- Whit Bissell - Prof. Harvey Glomm
- Peter Lorre Jr. - Transom
- Charles Horvath - Servant
- Craig Shreeve - U.N.C.L.E. Radioman
- Tita Marsell - Flamenco Dancer
- Gene Roth - Cycle Repairman
- William H. O'Brien - Grandpa
- Woodrow Parfrey - Dr. Ansel Pertwee
- William Lanteau - Analyst
- Naomi Stevens - Madame Hecubah
- Jack Gordon - Man on Sidewalk (uncredited)
- Jeannine Riley - Andy Francis
- Jeannine Riley - Nina Lillette
- James Hong - Prince Phanong
- James Hong - Mr. Chang
- Larry D. Mann - Arnold Fairbanks
- Larry D. Mann - Blodgett
- Diane McBain - Contessa Margo De Fanzini
- Diane McBain - Joanna Lydecker
- Hal Taggart - Club Member (uncredited)
- Hal Taggart - Lab Technichan (uncredited)
- Hal Taggart - Commuter (uncredited)
- John Larch - Dr. Killman
- Jack Bannon - U.N.C.L.E. Agent
- Gil Lamb - Daddy Jo
- Joe Mantell - Buuder
- Joe Mantell - L. C. Carson
- Richard Reeves - Crew Manager
- Norman Leavitt - Hiram
- Dub Taylor - Preacher
- Charles Seel - Uncle Charlie
- Charles Seel - Harry Baxter
- Burt Brinckerhoff - Chuck Boskirk
- Brooke Bundy - Terry Brent
- Elizabeth Allen - Carla Drosten
- Alfred Shelly - Guard
- Alfred Shelly - Angelo
- J. Carrol Naish - Uncle Giuliano
- John Harmon - Harry
- Alan Mowbray - Harry Blackburn
- Percy Rodriguez - President Khufu
- Jill Ireland - Imogen Smythe
- Jill Ireland - Marion Raven
- Raymond St. Jacques - Arunda
- Harold Gould - Doctor
- Eve Arden - Professor Lillian Stemmler
- Sharon Farrell - Sandy Wister
- Sharon Farrell - Jacqueline Midcult
- Sharon Farrell - Leslie Stemmler
- Buddy Lewis - THRUSH Agent
- Kamala Devi - Deirdre Purbhani
- George Sanders - G. Emory Partridge
- Jeanette Nolan - Edith Partridge
- John Alderson - Jenkins
- Nancy Kovack - Victoria Pogue
- James Doohan - Phillip Bainbridge
- James Doohan - Mr. MacInernay
- Michael St. Clair - Olaf
- Michael St. Clair - James
- Michael St. Clair - Knox
- Damian O'Flynn - Gentleman
- Madge Blake - Woman Tourist
- Madge Blake - Miriam Baxter
- Joan Collins - Baroness Bibi De Chasseur / Rosy Shlagenheimer
- Carl Esmond - Baron Freddy De Chasseur
- Chuck Hicks - Hans
- Chuck Hicks - Guard (uncredited)
- Pamela Curran - Inga Bergstrom
- Pamela Curran - Margo Hayward
- Paul Smith - Charlie
- Dorothy Neumann - Miss Pruit
- Vince Deadrick Sr. - Tommy Blenman
- Ted White - Assassin
- Jan Murray - Simon Sweet
- David Sheiner - Parviz
- David Sheiner - Walter Longolius
- David Sheiner - The Inspector
- Robert Emhardt - Colonel Picks
- Robert Emhardt - Heinrich Beckman
- Angelo Rossitto - Blind Pencil Seller
- Henry Jones - Vincent Lockridge
- Jeremy Slate - Gabe Melcroft
- Marta Kristen - Felicia Lavimore
- Ron Nyman - Driver (uncredited)
- Ron Nyman - Assassin (uncredited)
- Ron Nyman - Party Guest (uncredited)
- Alexander Lockwood - Jonas Wyatt Lavimore
- John Banner - Dr. Foster
- Dick Cherney - Thrush Agent (uncredited)
- Dick Cherney - Commuter at Airport (uncredited)
- Charles Dierkop - Adolph
- Lennie Weinrib - Winky Blintz
- Linda Marsh - Kyra
- Harold J. Stone - Stavros Macropalous
- Allen Jenkins - Enzo 'Pretty' Stilletto
- Joan Blondell - Mrs. Fingers Stilletto
- Penny Santon - Grandmama Monteri
- Frank Puglia - Padre Francisco
- Warren Parker - Second Passenger
- Caryl Lincoln - Wedding Guest (uncredited)
- George Sawaya - Thuggee
- George Sawaya - Tribesman
- George Sawaya - Hans
- George Sawaya - Henchman (uncredited)
- George Sawaya - Guard (uncredited)
- Robert Culp - Captain Shark
- Sue Ane Langdon - Elsa Barnman
- Herbert Anderson - Harry Barnman
- Hedley Mattingly - Captain Fowler
- J. Pat O'Malley - Francis X. O'Reilly
- J. Pat O'Malley - The Old Prospector
- Kent Smith - Mr. Macy
- Leon Belasco - Maxim Radish
- Leonid Kinskey - Ferenc Pifnic
- Linden Chiles - Tom Simpson
- Rex Holman - Eddie
- Rex Holman - Oregano
- Murray Matheson - The Maharajah
- Willard Sage - Duncan Bruce MacAlister
- Angela Lansbury - Elfie van Donck
- Danielle De Metz - Yvonne
- Fred Stromsoe - Karate Killer
- Arthur Tovey - Ship Passenger (uncredited)
- Arthur Tovey - Townsman (uncredited)
- Arthur Tovey - Office Spectator (uncredited)
- Arthur Tovey - Fencing Match Spectator (uncredited)
- Philip Ahn - Dr. Sazami Kyushu
- Horst Ebersberg - Swen
- Lynn Loring - Christine Hobson
- Lynn Loring - Neila Nillson
- Craig Chudy - Thrush Agent
- George Savalas - Greek Merchant
- Phyllis Newman - Sophie
- Michael Ansara - Sulador
- Carol Lynley - Annie Justin
- Peter Brocco - Dr. A.C. Nillson
- Peter Brocco - Dr. Segal
- Lola Albright - Azalea
- John Dehner - Dr. Parviz Kharmusi
- H.M. Wynant - Hassan Aksoy
- H.M. Wynant - Hassan Aksoy / Omar Aksoy / Karim Aksoy / Ali Aksoy
- Julie London - Laura Sebastian
- Lloyd Kino - Gardener
- Gene Raymond - Col. Allan Morgan
- Jack Donner - Premier Karim
- Anne Francis - Gervaise Ravel
- Richard Donner - Inebriate
- Rip Torn - Alexander
- Dorothy Provine - Tracey Alexander
- Norman Felton
- Sam Rolfe
Naomi Stevens interpreta a Madame Hecubah en la serie.
Leonid Kinskey hace el papel de Ferenc Pifnic.
George Sanders hace el papel de G. Emory Partridge.
Ted de Corsia interpreta a Chief Highcloud en la serie.
Martin Landau hace el papel de Count Ladislaus Zark.
Robert Ellenstein interpreta a Doctor Ieato en la serie.
Eve Arden interpreta a Professor Lillian Stemmler en la serie.
Sol Gorss interpreta a Konrad en la serie.
Vincent Price interpreta a Victor Marton en la serie.
Jack Palance interpreta a Louis Strago en la serie.
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