Hank Azaria

as Gargamel (voice)

Melissa Sturm

as Smurfette (voice)

Frank Welker

as Azrael (voice)

Anton Yelchin

as Clumsy Smurf (voice)

Tom Kane

as Narrator Smurf (voice)

Alan Cumming

as Gutsy Smurf (voice)

Fred Armisen

as Brainy Smurf (voice)

Jack Angel

as Papa Smurf (voice)

Adam Wylie

as Panicky Smurf (voice)

John Oliver

as Vanity Smurf (voice)

Gary Basaraba

as Hefty Smurf (voice)