 Francis MatthewsCaptain Scarlet (voice) | Captain Scarlet (voice) |
 Ed BishopCaptain Blue (voice) | Captain Blue (voice) |
 Donald GrayCaptain White / Captain Black / The Mysterons (voice) | Captain White / Captain Black / The Mysterons (voice) |
 Cy GrantLieutenant Green (voice) | Lieutenant Green (voice) |
 Elizabeth MorganDestiny Angel (voice) | Destiny Angel (voice) |
 Gary FilesCaptain Magenta / Pilot (voice) | Captain Magenta / Pilot (voice) |
 David HealyLunar Controller / Frazer (voice) | Lunar Controller / Frazer (voice) |
 Charles TingwellLieutenant Dean / Carter (voice) | Lieutenant Dean / Carter (voice) |
 Jeremy WilkinCaptain Ocher / Angelini / Control / Shroeder / Kurnitz / Human Captain Black (voice) | Captain Ocher / Angelini / Control / Shroeder / Kurnitz / Human Captain Black (voice) |
| MMartin KingOrson / Speech Intelligence Decoder (S.I.D.) (voice) | Orson / Speech Intelligence Decoder (S.I.D.) (voice) |
 Sylvia AndersonLinda Nolan / Receptionist (voice) | Linda Nolan / Receptionist (voice) |
 Paul MaxwellCaptain Grey / Breck (voice) | Captain Grey / Breck (voice) |
| JJanna Hill(voice) (credit only) | (voice) (credit only) |
| LLian-Shin Yang(voice) (credit only) | (voice) (credit only) |
