 Demi LovatoSmurfette (voice) | Smurfette (voice) |
 Rainn WilsonGargamel (voice) | Gargamel (voice) |
 Joe ManganielloHefty (voice) | Hefty (voice) |
 Jack McBrayerClumsy (voice) | Clumsy (voice) |
 Danny PudiBrainy (voice) | Brainy (voice) |
 Mandy PatinkinPapa Smurf (voice) | Papa Smurf (voice) |
 Julia RobertsSmurfwillow (voice) | Smurfwillow (voice) |
 Michelle RodriguezSmurfstorm (voice) | Smurfstorm (voice) |
 Ellie KemperSmurfblossom (voice) | Smurfblossom (voice) |
 Ariel WinterSmurflily (voice) | Smurflily (voice) |
 Meghan TrainorSmurfMelody (voice) | SmurfMelody (voice) |
 Jake JohnsonGrouchy (voice) | Grouchy (voice) |
 Dee Bradley BakerMonty (voice) | Monty (voice) |
 Frank WelkerAzrael (voice) | Azrael (voice) |
 Bret MarnellSnappy Bug / Handy Smurf (voice) | Snappy Bug / Handy Smurf (voice) |
 Brandon JeffordsCauldron (voice) | Cauldron (voice) |
 Kelly AsburyNosey Smurf (voice) | Nosey Smurf (voice) |
 Gabriel IglesiasJokey (voice) | Jokey (voice) |
 Tituss BurgessVanity (voice) | Vanity (voice) |
 Jeff DunhamFarmer (voice) | Farmer (voice) |
| PPatrick BallinPatient Smurf / Frank the Caterpillar (voice) | Patient Smurf / Frank the Caterpillar (voice) |
 Gordon RamsayBaker (voice) | Baker (voice) |
 Melissa SturmSmurfJade (voice) | SmurfJade (voice) |
 Alan MechemPasserby Smurf (voice) | Passerby Smurf (voice) |
| DDanik ThomasKarate Smurf (voice) | Karate Smurf (voice) |
 Eric BauzaAdditional Voices (voice) | Additional Voices (voice) |
 Ashley BellAdditional Voices (voice) | Additional Voices (voice) |
 Bob BergenAdditional Voices (voice) | Additional Voices (voice) |
 Debi DerryberryAdditional Voices (voice) | Additional Voices (voice) |
 Terri DouglasAdditional Voices (voice) | Additional Voices (voice) |
