Hank Azaria as Gargamel

Neil Patrick Harris as Patrick Winslow

Jayma Mays as Grace Winslow

Jonathan Winters as Papa Smurf (voice)

Katy Perry as Smurfette (voice)

Anton Yelchin as Clumsy Smurf (voice)

Sofía Vergara as Odile Anjelou

Tim Gunn as Henri

Frank Welker as Azrael (voice)

Madison McKinley as Model

Meg Phillips as Model

Mahadeo Shivraj as Cabbie

Julie Chang as Newscaster

Mark Doherty as Bluetooth Businessman

Minglie Chen as Young Woman

Sean Kenin as Guy in Plaid Shirt

Victor Pagan as Bum

Adria Baratta as Anjelou Employee

Paula Pizzi as Odile's Mother

Andrew Sellon as Waiter

Julianna Rigoglioso as Little Sister

Daria Rae Figlo as Blonde Sister

Bradley Gosnell as Toy Salesperson

Heidi Armbruster as Toy Store Parent

Finnerty Steeves as Toy Store Parent

John Speredakos as Parent with Girls

Skai Jackson as Kicking Girl

Alex Hall as Skateboard Kid

Eric Redgate as Skateboard Kid

Jojo Gonzalez as FAO Custodian

Scott Dillin as Cop

Tyree Michael Simpson as Cop

Sean Ringgold as Inmate Bubba

Mario D'Leon as Bubba's Inmate Friend

Liz Smith as Party Guest

Tom Colicchio as Party Guest

Michael Musto as Party Guest

Joan Rivers as Party Guest

Olivia Palermo as Party Guest

Julia Enescu as Party Guest

Lauren Waggoner as Party Guest

Mr. Krinkle as Azrael

Hank as Elway

Alan Cumming as Gutsy Smurf (voice)

Fred Armisen as Brainy Smurf (voice)

George Lopez as Grouchy Smurf (voice)

Kenan Thompson as Greedy Smurf (voice)

Jeff Foxworthy as Handy Smurf (voice)

John Oliver as Vanity Smurf (voice)

Wolfgang Puck as Chef Smurf (voice)

Gary Basaraba as Hefty Smurf (voice)

Paul Reubens as Jokey Smurf (voice)

B.J. Novak as Baker Smurf (voice)

Tom Kane as Narrator Smurf (voice)

John Kassir as Crazy Smurf (Voice)

Joel McCrary as Farmer Smurf (voice)

Mary McGloin as Mother of Girl in Store (uncredited)