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| Maxwell Smart: | Don Adams |
| Agent 99: | Barbara Feldon |
| Thaddeus, The Chief: | Edward Platt |
| Conrad Siegfried, head of KAOS: | Bernie Kopell |
| Agent 44: | Victor French |
| Admiral Harold Harmon Hargrade: | William Schallert |
| Dr. Steele, head of lab: | Ellen Weston |
| Hymie, CONTROL robot: | Dick Gautier |
| Charlie Watkins, CONTROL agent: | Angelique Pettyjohn |
| Professor Windish, scientist: | Robert Cornthwaite |
| Charlson, scientist: | Stacy Keach, Sr. |
| Dr. Bascomb, head of crime lab: | George Ives |
| Starker, Siegfried's aide: | King Moody |
| 99's mother: | Jane Dulo |
| Agent 13: | David Ketchum |
| Harry Hoo, detective: | Joey Forman |


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