Robert Vaughn
Napoleon Solo (16 eps)
David McCallum
Illya Kuryakin (16 eps)
Leo G. Carroll
Alexander Waverly (16 eps)
Susan Odin
Melissa Hargrove (1 eps)
Charles McGraw
Jules Cutter (1 eps)
Charles Drake
Taggart Coleman (1 eps)
Nobu McCarthy
Monica Hyodo (1 eps)
Robert Ellenstein
Doctor Ieato (1 eps)
Charles H. Radilak
Ambassador Vanderloon (as Charles H. Radilac) (1 eps)
Eric Feldary
Kramer (1 eps)
Jacqueline Dalya
Countess (1 eps)
Karen Carlson
Helene (1 eps)
Sid Haig
Alex (1 eps)
Larry Anthony
Commander Jenkins (1 eps)
John Larch
Dr. Killman (1 eps)
Jack Bannon
U.N.C.L.E. Agent (1 eps)
Hal Taggart
Lab Technichan (uncredited) (1 eps)