- Neil Patrick Harris Character (Patrick Winslow)
- Christina Ricci Character (Vexy)
- Katy Perry Character (Smurfette)
- Hank Azaria Character (Gargamel)
- Brendan Gleeson Character (Victor)
- Alan Cumming Character (Gutsy Smurf)
- Jayma Mays Character (Grace)
- Jonathan Winters Character (Papa Smurf)
- J. B. Smoove Character (Hackus)
- George Lopez Character (Grouchy Smurf)
- Anton Yelchin Character (Clumsy Smurf)
- John Oliver Character (Vanity Smurf)
- Jacob Tremblay Character (Blue)
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