Characters played by Jack Angel
Papa
Characters played by Fred Armisen
Brainy
Characters played by Hank Azaria
Gargamel
Characters played by Gary Basaraba
Hefty
Characters played by George Lopez
Grouchy
Characters played by Melissa Sturm
Smurfette
Characters played by Anton Yelchin
Clumsy
Characters played by Frank Welker
Azrael