The two-time Emmy Award winner has been scoring the music on the popular animated series for the past 27 years, but he claims to have been given his marching orders.
Alf has told Variety that he received a phone call from producer Richard Sakai who informed him he would no longer be scoring the Fox show because the company are seeking a "different kind of music".
The 76-year-old composer has scored more than 560 episodes of the series and has received 23 Emmy nominations for The Simpsons, including his two victories in 1997 and 1998. He has also received seven nods for other projects, and won five Annie Awards for his work on the show.
Alf scored season 28 of The Simpsons, which aired in May, but it's not known if he will be the music man on series 29 when it kicks off on October 1st. However, Danny Elfman's famous Simpsons theme song is expected to be retained by Fox.
A Fox spokeswoman declined to comment to the publication.
This comes two years after Harry Shearer - the voice of Mr. Burns, Ned Flanders, Principal Skinner and several other characters - announced he was leaving the show, but two months later he reversed his decision.
He was said to have signed a four-season deal worth a reported $300,000 per episode. The Simpsons first aired in December 1989 and has run for more than 600 episodes.
- Emmy-nominated "Vote for a Winner" (from "The President Wore Pearls"): From the great opening joke by lyricist Dana Gould - "J'accuse, Monsieur Cusperberg!" - Yeardley Smith's Lisa really delivers in this "Evita" parody.
- "Union Strike Folk Song (Parts 1 and 2)" (from "Last Exit to Springfield"): "They have the plant / But we have the power." Lisa may be best known for her jazz, but she channels the best protest folkies of yore - and shows off some sweet six-string chops.
- "Dr. Zauis/Chimpan A to Chimpan Z" (from "A Fish Called Selma"): With Troy McClure as the production's Charlton Heston, this music nods to both the Broadway musical "Stop the World, I Want to Get Off" and Falco's "Rock Me Amadeus," with breakdancing thrown in for humorous measure.
- "See My Vest" (from "Two Dozen and One Greyhounds"): "Like my loafers? Former gophers!" The gleeful villainy of Monty Burns plays brilliantly in this dark spoof of "Beauty and the Beast."
- "The Monorail Song" (from "Marge vs. the Monorail"): Showrunner Al Jean and a young Conan O'Brien helped pen this brilliant "Music Man" send-up.
- Emmy-winning "We Put the Spring in Springfield" (from "Bart After Dark"): The kind of big production number - co-written by "Futurama" creative force Ken Keeler - that surely inspired MacFarlane years before his own animated show.
- Emmy-nominated "Always My Dad" (from "A Star Is Torn"): Lisa Simpson wrote this talent-show tune at the last minute, but clearly Clausen and Carolyn Omine put some real time into crafting it.
- Emmy-winning "You're Checkin' In" from the musical "Kickin' It" (from "The City of New York vs. Homer Simpson"): "I should put you away where you can't kill or maim us, but this is L.A., and you're rich and famous!" This finger-snapping tune offers some of the sharpest lyrics in a musical journey through the Betty Ford Center.
- Emmy-nominated "Señor Burns" (from "Who Shot Mr. Burns? (Part 2)"): When you can land the real Latin jazz legend Tito Puente, you go to town musically with it. "Adios viejo!"
- Emmy-nominated "Ode to Branson" (from "The Old Man and the Key"): Fun fact: This star-studded revue tune lost the Emmy to then-upstart Fox stablemate "Family Guy."
- "Canyonero" (from "The Last Temptation of Krust"): Some of the show's very best skewering of Madison Avenue as the '90s SUV craze took hold.
- "The Amendent Song" (from "The Day the Violence Died"): A "Schoolhouse Rock" parody so on point that the "Simpsons" producers even got original warbler Jack Sheldon to sing this spoof.
As well as The Simpsons, Alf has scored more than 30 movies and TV shows, such as Ferris Bueller's Day Off, The Naked Gun, Moonlighting and ALF.