 Lucille BlissSmurfette (voice) | Smurfette (voice) |
 Charlie AdlerNatural 'Nat' Smurfling / Thief (voice) | Natural 'Nat' Smurfling / Thief (voice) |
 William CallawayClumsy Smurf / Rich Man (voice) | Clumsy Smurf / Rich Man (voice) |
 Hamilton CampGreedy Smurf (voice) | Greedy Smurf (voice) |
 Julie McWhirterBaby Smurf / Sassette Smurfling (voice) | Baby Smurf / Sassette Smurfling (voice) |
 Jeff DoucetteSheriff (voice) | Sheriff (voice) |
 Bernard ErhardTimber Smurf (voice) | Timber Smurf (voice) |
 June ForayJokey Smurf (voice) | Jokey Smurf (voice) |
 Justin GockeHans (voice) | Hans (voice) |
 Danny GoldmanBrainy Smurf (voice) | Brainy Smurf (voice) |
| KKip KingTailor Smurf (voice) | Tailor Smurf (voice) |
 Don MessickPapa Smurf / Chitter (voice) | Papa Smurf / Chitter (voice) |
 Pat MusickSnappy Smurfling / Anna (voice) | Snappy Smurfling / Anna (voice) |
 Noelle NorthSlouchy Smurfling (voice) | Slouchy Smurfling (voice) |
 Alan OppenheimerVanity Smurf / Doctor (voice) | Vanity Smurf / Doctor (voice) |
 William SchallertWillem (voice) | Willem (voice) |
 Les TremayneGustav (voice) | Gustav (voice) |
 Peggy WebberElise (voice) | Elise (voice) |
 Frank WelkerHefty Smurf / Poet Smurf / Wild Smurf / Puppy / Rat (voice) | Hefty Smurf / Poet Smurf / Wild Smurf / Puppy / Rat (voice) |
 Jonathan WintersGrandpa Smurf (voice) | Grandpa Smurf (voice) |
