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Madison McKinley as Model Hank Azaria as Gargamel Jayma Mays as Grace Winslow Tim Gunn as Henri John Speredakos as Parent with Girls Mario D'Leon as Bubba's Inmate Friend Michael Musto as Party Guest Mahadeo Shivraj as Cabbie Mary McGloin as Mother of Girl in Store (uncredited) Neil Patrick Harris as Patrick Winslow B. J. Novak as Baker Smurf (voice) John Oliver as Vanity Smurf (voice) Gary Basaraba as Hefty Smurf (voice) Andrew Sellon as Waiter Wolfgang Puck as Chef Smurf (voice) Paul Reubens as Jokey Smurf (voice) Katy Perry as Smurfette (voice) Sean Ringgold as Inmate Bubba Tom Colicchio as Party Guest Jonathan Winters as Papa Smurf (voice) Sean Kenin as Guy in Plaid Shirt Jeff Foxworthy as Handy Smurf (voice) John Kassir as Crazy Smurf (Voice) Tom Kane as Narrator Smurf (voice) Scott Dillin as Cop Frank Welker as Azrael (voice) Joan Rivers as Party Guest Joel McCrary as Farmer Smurf (voice) Anton Yelchin as Clumsy Smurf (voice) Meg Phillips as Model Fred Armisen as Brainy Smurf (voice) Paula Pizzi as Odile's Mother Bradley Gosnell as Toy Salesperson Heidi Armbruster as Toy Store Parent Skai Jackson as Kicking Girl Minglie Chen as Young Woman Jojo Gonzalez as FAO Custodian Sofía Vergara as Odile Anjelou Mark Doherty as Bluetooth Businessman Victor Pagan as Bum Julianna Rigoglioso as Little Sister Alan Cumming as Gutsy Smurf (voice) Kenan Thompson as Greedy Smurf (voice) Liz Smith as Party Guest Olivia Palermo as Party Guest George López as Grouchy Smurf (voice)

Jill Brown Stunts Raja Gosnell Director Adam Hlavac Visual Effects Peyo Characters, Comic Book Chris Cenatiempo Stunts Sabrina Plisco Editor Aja Frary Stunts Rita Ryack Costume Design Ronni Brown Foley Artist Shawnna Thibodeau Stunts Heitor Pereira Original Music Composer Bill Boes Production Design John Cenatiempo Stunts Richard Hicks Casting Todd Tucker Makeup Designer Phil Meheux Director of Photography