- Neil Patrick Harris Character (Patrick Winslow)
- Jayma Mays Character (Grace Winslow)
- Anton Yelchin Character (Clumsy Smurf)
- Hank Azaria Character (Gargamel)
- Alan Cumming Character (Gutsy Smurf)
- Katy Perry Character (Smurfette)
- Sofa Vergara Character (Odile)
- Jonathan Winters Character (Papa Smurf)
- George Lopez Character (Grouchy Smurf)
- Paul Reubens Character (Jokey Smurf)
- Kenan Thompson Character (Greedy Smurf)
- B. J. Novak Character (Baker Smurf)
- Jeff Foxworthy Character (Handy Smurf)
- Wolfgang Puck Character (Chef Smurf)
- Fred Armisen Character (Brainy Smurf)
- John Oliver Character (Vanity Smurf)
- Adam Wylie Character (Panicky Smurf)
- Gary Basaraba Character (Hefty Smurf)
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