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Demi Lovato - Smurfette (voice) , Rainn Wilson - Gargamel (voice) , Joe Manganiello - Hefty Smurf (voice) , Jack McBrayer - Clumsy Smurf (voice) , Danny Pudi - Brainy Smurf (voice) , Mandy Patinkin - Papa Smurf (voice) , Dee Bradley Baker - Monty (voice) , Frank Welker - Azrael (voice) , Michelle Rodriguez - SmurfStorm (voice) , Ellie Kemper - SmurfBlossom (voice) , Julia Roberts - SmurfWillow (voice) , Ariel Winter - SmurfLily (voice) , Meghan Trainor - SmurfMelody (voice) , Bret Marnell - Snappy Bug / Handy Smurf (voice) , Brandon Jeffords - Cauldron (voice)