Jack Angel as Papa Smurf (voice)

Fred Armisen as Brainy (voice)

Hank Azaria as Gargamel (voice)

Gary Basaraba as Hefty (voice)

George López as Grouchy (voice)

Melissa Sturm as Smurfette (voice)

Anton Yelchin as Clumsy (voice)

Frank Welker as Azrael (voice)

Kirk Baily as Additional Voices (voice)

Jess Harnell as Additional Voices (voice)

Jeff Fischer as Additional Voices (voice)

Craig Kellman as Additional Voices (voice)

John Hans Tester as Additional Voices (voice)