Some of the Smurfs, including Papa Smurf and Brainy, appeared along with Baby Kermit, Baby Piggy, and Baby Gonzo in the 1990 animated television special Cartoon All-Stars to the Rescue. They had previously appeared in a 1987 comic-style print ad, with the cast of the animated Fraggle Rock and other NBC characters in the commissary.
- In The Smurfs 2011 movie, an unauthorized Elmo walk-around is seen on the streets of New York, which the Smurfs believe is a red troll. The Muppet Whatnot Workshop is also seen in the background of another scene, when Gargamel is thrown out of the elevator at FAO Schwarz.
- In episode 205 of Muppets Tonight, Don Rickles is hired by Ernst Stavros Grouper to act as therapist and boost company morale. Rickles reports after having met with the Muppets: "I talked to your happy little Smurf friends."
- Fred Armisen voiced Brainy Smurf in the 2011 film
- Bob Arbogast provided guest voices
- Hank Azaria played Gargamel in the 2011 and 2013 films
- Gregg Berger provided guest voices
- Ruth Buzzi provided guest voices
- Alan Cumming voiced Gutsy Smurf in the 2011 film
- Jeff Foxworthy voiced Handy Smurf the 2011 film
- Skai Jackson played Kicking Girl in the 2013 film
- Neil Patrick Harris played Patrick Winslow in the 2011 and 2013 films
- Ellie Kemper voiced Smurfblossom in Smurfs: The Lost Village (2017)
- Jimmy Kimmel voiced Passive Aggressive Smurf in the 2013 sequel
- George Lopez voiced Grouchy Smurf in the 2011 film
- Mario Lopez voiced Social Smurf in the 2013 sequel
- Jack McBrayer voiced Clumsy Smurf in Smurfs: The Lost Village (2017)
- Edie McClurg provided guest voices
- Nancy O'Dell made a cameo as herself in the 2013 sequel
- John Oliver voiced Vanity Smurf in the 2011 film
- Rob Paulsen voiced Marco Smurf in the episode "Marco Smurf and the Pepper Pirates"
- Katy Perry voiced Smurfette in the 2011 and 2013 films.
- Gordon Ramsay voiced Baker Smurf in Smurfs: The Lost Village (2017)
- Paul Reubens voiced Jokey Smurf in the 2011 film
- Cliff Roberts was a staff writer on the Hanna-Barbera series
- Wolfgang Puck voiced Chef Smurf in the 2011 film
- Joan Rivers appeared as herself in the 2011 film
- Will Ryan voiced one of the Wartmongers (1981-1989)
- William Schallert provided guest voices on the series and voiced Willem in the special Tis the Season to Be Smurfy (1987)
- John Stephenson provided guest voices
- Fred Travalena provided guest voices
- Russi Taylor voiced Smoogle (1988-1990)
- Jacob Tremblay played Blue Winslow in the 2013 film
- Sofia Vergara played Odile in the 2011 film
- Frank Welker voiced Hefty Smurf, Peewit, Poet Smurf, Clockwork Smurf, Puppy, Wild Smurf, and others. He also voiced Azrael in the 2011 and 2013 films
- Jonathan Winters voiced Grandpa Smurf (1985-1990) and Papa Smurf in the 2011 and 2013 films
- William Woodson provided guest voices