 | Hank Azaria als Gargamel |
 | Neil Patrick Harris als Patrick Winslow |
 | Jayma Mays als Grace Winslow |
 | Brendan Gleeson als Victor Doyle |
 | Katy Perry als Smurfette (voice) |
 | Jacob Tremblay als Blue Winslow |
 | Nancy O'Dell als Nancy O'Dell |
 | Karim Babin als Room Service Waiter |
 | Gaston Morrison als New York Taxi Driver |
 | Jocelyn Blanchard als Toad Man |
 | Erika Rosenbaum als Pregnant Mom |
 | Carolina Bartczak als Peanut Mom |
 | James A. Woods als Peanut Father |
 | Henri Pardo als Father-to-Be |
 | Vanessa Matsui als Mother with Camera |
 | Dusan Dukic als Curious Dad |
 | Ruth Chiang als Single Mom |
| Andy Quesnel als Woman in Box |
 | Mylène Dinh-Robic als Hotel Assistant Manager |
| Martin-Guy Bélanger als Hotel Sous-chef |
| Robert Reynaert als Candy Man |
 | Patrick Sabongui als Candy Man |
| Martin St-Antoine als Tourist with Coffee Cup |
 | Patrick Baby als Palais Garnier Security Guard |
| Joshua Spreekmeester als Peanut Kid |
 | Bruno Paviot als Hotel Desk Manager |
| Gunther Love als Cat Man in Audience |
 | Gaëlle Pietri als Pregnant Model (as Gaelle Herisson Pietri) |
 | Janicke Askevold als Pregnant Model |
 | Beatrice Rosen als Pregnant Model |
| Mathilde Snodgrass als Pregnant Model |
| Mr. Krinkle als Azrael |
| Hank als Elway |
 | Christina Ricci als Vexy (voice) |
 | Jonathan Winters als Papa Smurf (voice) |
 | J.B. Smoove als Hackus (voice) |
 | George Lopez als Grouchy Smurf (voice) |
 | Anton Yelchin als Clumsy Smurf (voice) |
 | John Oliver als Vanity Smurf (voice) |
 | Frank Welker als Azrael (voice) |
 | Tom Kane als Narrator Smurf (voice) |
 | Fred Armisen als Brainy Smurf (voice) |
 | Jeff Foxworthy als Handy Smurf (voice) |
 | Alan Cumming als Gutsy Smurf (voice) |
 | Gary Basaraba als Hefty Smurf (voice) |
 | Adam Wylie als Panicky Smurf (voice) |
 | Joel McCrary als Farmer Smurf (voice) |
 | Kenan Thompson als Greedy Smurf (voice) |
 | Kevin Lee als Party Planner Smurf (voice) |
 | Paul Reubens als Jokey Smurf (voice) |
 | Shaquille O'Neal als Smooth Smurf (voice) |
 | B.J. Novak als Baker Smurf (voice) |
 | Jimmy Kimmel als Passive-Aggressive Smurf (voice) |
 | Shaun White als Clueless Smurf (voice) |
 | Mario López als Social Smurf (voice) |
 | John Kassir als Crazy Smurf (voice) |
 | Sean Kenin als Smurf Voice #1 (voice) |
 | Patricia Summersett als Smurf Voice #2 (voice) |
| Michael Parks | Animation |
| Juan Miguel Vadell | Animation |
| Wayne Jaworskyj | Compositors |
| Jacob Jared Jones | Compositors |
| Jessica Wolff | Compositors |
| Dixie Pizani | Animation |
| Aaron Williams | VFX Artist |
| David Settlow | Visual Effects Design Consultant |
| Elizabeth McClurg | Compositors |
| Joo-Hwan Park | Compositors |
| Karey Kirkpatrick | Screenplay |
| David Ronn | Story |
| David N. Weiss | Story |
| David N. Weiss | Screenplay |
| Jay Scherick | Story |
| Benita Allen | Co-Producer |
| J. David Stem | Story |
| Jay Scherick | Screenplay |
| Ben Haber | Executive Producer |
| David Ronn | Screenplay |
| Raphaël Benoliel | Co-Producer |
| Hendrik Coysman | Co-Producer |
| Véronique Culliford | Co-Producer |
| Peyo | Characters |
| Carole Schmidlin Blanchard | Crowd Assistant Director |
| Paul Neesan | Executive Producer |
| Frédérique Bolté | Set Decoration |
| Jordan Kerner | Producer |
| Juliette Ménager | Casting |
| Marie-Soleil Dénommé | Set Decoration |
| Véronique Marchessault | Costume Design |
| Sarah Heitz de Chabaneix | Additional Third Assistant Director |
| Sabrina Plisco | Associate Producer |
| Benoît Tetelin | Set Decoration |
| Michael Killoren | Production Manager |
| G. A. Aguilar | Second Unit Director |
| Dominic Gaglione D'Amico | Third Assistant Director |
| Silver Butler | Second Second Assistant Director |
| Martin Doepner | Additional Third Assistant Director |
| Ezra Swerdlow | Executive Producer |
| Nancy Honeycutt | Production Supervisor |
| Yannick Fauchier | Second Assistant Director |
| Andrea Kenyon | Casting |
| David Rubin | Casting |
| Geoffroy Gosselin | On Set Dresser |
| Matthieu Rubin | Unit Production Manager |
| Gabrielle Hanne | Second Assistant Director |
| Sabrina Plisco | Editor |
| David Gaucher | Art Direction |
| Anaïs Barrat | Crowd Assistant Director |
| Maxence Paris | Crowd Assistant Director |
| David E. Hall | Post Production Supervisor |
| Yann Le Boucher | Third Assistant Director |
| Michele Laliberte | Supervising Art Director |
| Benita Allen | First Assistant Director |
| Phil Meheux | Director of Photography |
| Bill Boes | Production Design |
| Daniel Carbo | Production Manager |
| Ariane Côté-Chénier | Additional Third Assistant Director |
| Maricel Pagulayan | Associate Producer |
| Pascale Deschênes | Set Decoration |
| Paul Boutin | Unit Manager |
| Felix Baudouin | Second Assistant Director |
| Serena Yang | Second Unit Director |
| David Laramy | Set Decoration |
| Rita Ryack | Costume Design |
| Lea Lambert | Production Manager |
| Emma Pucci | Art Direction |
| Antoine Desanti | Assistant Director |
| Vincent Gingras-Liberali | Art Direction |
| Raja Gosnell | Director |
| Alain Moussi | Stunts |
| Randi Wells | Casting |
| Jered Zalman | Assistant Editor |
| Becky G | Songs |
| Austin Mahone | Songs |
| J. David Stem | Screenplay |
| Sinan Saber | Third Assistant Director |
| Peyo | Comic Book |
| Heitor Pereira | Original Music Composer |
| Todd Tucker | Makeup Department Head |
| G. A. Aguilar | Stunt Coordinator |
| Sean Dwyer | First Assistant Director |
| Matt Salkin | Visual Effects Coordinator |
