The film, based on the popular cartoon series, will be a hybrid of live-action and animation, directed by Raja Gosnell. Azaria will voice the villain Gargamel, and Mays will play the pregnant wife of previously announced cast member Neil Patrick Harris (Cabaret, Rent, Assassins). The pair will play the film's only human characters.

The cast of voices also includes the previously reported Tony winner Alan Cumming (Cabaret, The Threepenny Opera) as Gutsy Smurf, comedian George Lopez as Grouchy Smurf, actor/director Quentin Tarantino as Brainy Smurf and pop star Katy Perry as Smurfette.

Azaria, who appeared on Broadway in Spamalot and The Farnsworth Invention, is perhaps best known for his work on animated series "The Simpsons." He is the voice of Chief Wiggum, Kwik-E-Mart owner Apu, and bar owner Moe, among many others. His film credits include "The Birdcage," "Dodgeball" and "Cradle Will Rock," in which he played Broadway composer Marc Blitzstein.

Mays currently stars as guidance counselor Emma Pillsbury on the hit television show "Glee." Her previous television credits include roles on "Heroes" and "Ugly Betty."

Filming is currently underway for "The Smurfs," and the film is scheduled for release in 2011.