•
Charlie Adler as Nat Smurfling, Glut (in "Clumsy's Cloud"), Grogg (in "The Smurfs That Time Forgot") •
Jack Angel as Enchanter Homnibus, Additional voices • Marlene Aragon as Additional voices •
Bob Arbogast as Additional voices •
Lewis Arquette as Additional voices •
René Auberjonois as Additional voices •
Jered Barclay as Additional voices • Bernard Behrens as Additional voices •
Michael Bell as Grouchy Smurf, Handy Smurf, Lazy Smurf,
Johan, Painter Smurf (in "The Hundredth Smurf"), Gargamel (Season 9), Additional voices •
Gregg Berger as Additional voices •
Joe Besser as
Cupid •
Lucille Bliss as
Smurfette •
Susan Blu as Nanny Smurf, Pansy •
Sorrell Booke as Additional voices • Peter Brooks as Additional voices •
Greg Burson as Additional voices •
Ruth Buzzi as Additional voices •
William Callaway as Clumsy Smurf, Painter Smurf, Don Smurfo, Additional voices •
Joey Camen as Natural Smurf (adult form) •
Hamilton Camp as Greedy Smurf, Harmony Smurf, Woody, Additional voices •
Roger C. Carmel as Additional voices •
Victoria Carroll as Additional voices •
Mary Jo Catlett as Madame Hildegarde (in "Stop and Go Smurfs") •
William Christopher as Angel Smurf •
Philip L. Clarke as Additional voices • Selette Cole as Additional voices •
Townsend Coleman as Additional voices •
Henry Corden as Grako (in "The Magic Fountain") •
Regis Cordic as Additional voices •
Peter Cullen as
Zeus (in "The Smurf Odyssey"), Gluttonous the Gourmet (in "A Fish Called Snappy"), Additional voices •
Brian Cummings as Additional voices •
Jim Cummings as the Sultan of Sweets (in "Sky High Surprise") •
Keene Curtis as Lord Balthazar •
Jennifer Darling as Princess Sabina, Additional voices •
Leo De Lyon as Additional voices •
Barry Dennen as Additional voices • Bronwen Denton-Davis as Additional voices •
Patti Deutsch as Bignose, Additional voices •
Walker Edmiston as Additional voices •
Marshall Efron as Sloppy Smurf •
Paul Eiding as Additional voices •
Richard Erdman as Additional voices •
Bernard Erhard as Timber Smurf •
June Foray as Jokey Smurf,
Mother Nature, Gargamel’s mother, Additional voices •
Pat Fraley as Tuffy Smurf, Additional voices •
Teresa Ganzel as Additional voices •
Linda Gary as Dame Barbara, Chlorhydris (all episodes except the special "My Smurfy Valentine") •
Dick Gautier as Wooly Smurf •
Joan Gerber as Priscilla (in "The Tear of a Smurf"), Gowagga Puppet (in "Snappy's Puppet"), Additional voices •
Henry Gibson as Additional voices •
Ed Gilbert as Additional voices • Patty Glick as Additional voices •
Danny Goldman as Brainy Smurf •
Barry Gordon as the Gamemaster (in "The Grouchiest Game in Town") • Joy Grdnic as Additional voices • Ernest Harada as Additional voices •
Phil Hartman as Additional voices •
Billie Hayes as Drusilla (in "Chlorhydris’s Lost Love") •
Bob Holt as the Good King •
Jerry Houser as Ripple (in "The Smurflings' Unsmurfy Friend"), Tebuli the Genie (in "The Clumsy Genie"), Additional voices •
John Ingle as Additional voices •
Robert Ito as Additional voices •
Tony Jay as
Merlin (in "The Smurfs of the Round Table") •
Arte Johnson as Devil Smurf •
Marvin Kaplan as Gourdy (in "Farmer's Genii", "The Tallest Smurf", and "Master Scruple") • Zale Kessler as Additional voices •
Aron Kincaid as Additional voices •
Kip King as Tailor Smurf • Paul Kirby as Additional voices •
Clyde Kusatsu as Additional voices •
Robbie Lee as Additional voices •
Ruta Lee as Evelyn (in "Gargamel's Sweetheart"),
Morgan le Fay (in "The Smurfs of the Round Table") •
Katie Leigh as Denisa (in "A Smurf for Denisa", "Denisa's Greedy Doll", and "Denisa's Slumber Party") •
Michael Lembeck as Additional voices •
Marilyn Lightstone as Additional voices •
Keye Luke as Additional voices •
Allan Lurie as Additional voices •
Jim MacGeorge as Additional voices •
Norma MacMillan as Brenda (in "The Littlest Witch") •
Tress MacNeille as Simon (in "The Littlest Giant"), Sylvia (in "The Smurf Odyssey"), Additional voices •
Patty Maloney as Blue Eyes (in "The Little Orange Horse with the Gold Shoes" and "Blue Eyes Returns") • Danny Mann as Additional voices •
Kenneth Mars as King Bullrush, Julius Geezer (in "Gnoman Holiday"), Additional voices •
Mona Marshall as Weepy Smurf, Flowerbell (in "Papa's Wedding Day"), Andria (in "Wedding Bells for Gargamel") •
Amanda McBroom as Chlorhydris (in the special "My Smurfy Valentine"), Additional voices •
Chuck McCann as Additional voices •
Julie McWhirter as Baby Smurf, Sassette Smurfling •
Allan Melvin as Dufus the Giant (in "Gargamel's Giant"), Additional voices •
Don Messick as Papa Smurf, Azrael, Dreamy Smurf, Chitter the Squirrel, Sickly Smurf, Sweepy Smurf, Additional voices •
Sidney Miller as Additional voices • Larry Moss as Additional voices • Janice Motoike as Additional voices •
Pat Musick as Snappy Smurfling •
Frank Nelson as Nosey Smurf, Additional voices • Noelle North as Slouchy Smurfling •
Alan Oppenheimer as Vanity Smurf,
Father Time, Additional voices •
Patricia Parris as Acorn •
Rob Paulsen as Marco Smurf, Additional voices • Clare Peck as Additional voices •
Diane Pershing as Additional voices •
Brock Peters as the Ambassador of Zad (in "The Moor’s Baby") •
Patrick Pinney as Additional voices •
Henry Polic II as Tracker Smurf, Keswick (in "Legendary Smurfs"), Additional voices •
Philip Proctor as King Gerard •
Clive Revill as Additional voices •
Robert Ridgely as Additional voices •
Neil Ross as Additional voices •
Joseph Ruskin as Additional voices •
Will Ryan as Slime the Wartmonger, Anton (in "Legendary Smurfs") •
Michael Rye as Morlock (in "The Prince and the Hopper" and "Gargamel's New Job"), Additional voices •
Bob Sarlatte as Additional voices •
Ronnie Schell as Pushover Smurf, Reporter Smurf, Jokey Smurf (in "The Smurfette" and "Vanity Fare"), Dreamy Smurf (in "The Astrosmurf"), Additional Voices •
Marilyn Schreffler as Additional voices •
Avery Schreiber as Additional voices •
Franklin Seales as Additional voices •
Susan Silo as Petaluma (in "Smurfette's Flower"), Additional voices •
Hal Smith as Sludge the Wartmonger, Dismal Boggs (in "The Secret of Shadow Swamp"), Additional voices •
Kath Soucie as Adella (in "Stop and Go Smurfs"), Ali Baby (in "Sky High Surprise"), Additional voices •
John Stephenson as the Treasure Hunter Imp and the Spirit of the Ancient Trolls (in "Smurfette's Dancing Shoes"), Malakov (in "Dancing Bear" and "I Was a Brainy Weresmurf"), Additional voices • Kris Erik Stevens as Additional voices • Alexandra Stoddart as Additional voices •
Andre Stojka as Additional voices • Dee Stratton as Additional voices •
George Takei as Additional voices •
Mark L. Taylor as Additional voices •
Russi Taylor as Smoogle, Brenda (in "Scruple's Sweetheart"), Additional voices •
Susan Tolsky as Additional voices •
Fred Travalena as Additional voices •
Marcelo Tubert as Additional voices •
Brenda Vaccaro as Scruple, Architect Smurf •
Janet Waldo as Hogatha •
Ray Walston as Additional voices •
Peggy Walton-Walker as Additional voices •
B. J. Ward as
Hermes (in "The Smurf Odyssey"), Additional voices •
Peggy Webber as Elderberry •
Lennie Weinrib as Bigmouth •
Frank Welker as Hefty Smurf, Clockwork Smurf, Peewit, Poet Smurf, Puppy, Wild Smurf, Nemesis,
Sandman, Additional voices •
Paul Winchell as
Gargamel (Season 1–8), Flighty Smurf, Additional voices •
Jonathan Winters as Grandpa Smurf • Francine Witkin as Lady Luck (in "Bad Luck Smurfs") • Anderson Wong as Additional voices • Michael Wong as Additional voices •
Alan Young as Farmer Smurf, Miner Smurf, Scaredy Smurf, Milton McKilty (in "Phantom Bagpiper"), Additional voices ==Production==