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It is not looking like an okely-dokely day in the town of Springfield: Harry Shearer, an Emmy Award-winning cast member of “The Simpsons,” who provides the voices of characters like the irritatingly upbeat neighbor Ned Flanders, the billionaire tyrant Mr. Burns and his faithful manservant, Smithers, has indicated that he is parting ways with this long-running Fox animated series.

[Quiz: Which “Simpsons” characters did Harry Shearer voice?]

Mr. Shearer, who has been a part of the “Simpsons” cast since it made its debut in 1989, wrote in a series of Twitter posts published overnight that his involvement with the show was coming to an end. He wrote that he had been told by a lawyer for James L. Brooks, a “Simpsons” executive producer, that the “show will go on, Harry will not be part of it, wish him the best.”

Mr. Shearer wrote that this occurred “because I wanted what we’ve always had: the freedom to do other work.” He added, “Of course, I wish him the very best.”

In another tweet, Mr. Shearer said, “Thanks, Simpsons fans, for your support.”

Al Jean, the “Simpsons” showrunner, said in an email, “Harry Shearer was offered the same deal the rest of the cast accepted, and passed. The show will go on and we wish him well. Maggie took it hard.”

Mr. Brooks, however, indicated that he is open to further negotiation with Mr. Shearer, tweeting, “Hey, we tried. We’re still trying. Harry, no kidding, let’s talk.”

Press representatives for Fox and “The Simpsons” did not immediately respond to requests for comment on Thursday morning.

Fox announced earlier this month that it had picked up “The Simpsons” for two more years – the show’s 27th and 28th seasons, which would bring it to more than 600 episodes.

Mr. Shearer, a comedian and actor who also appeared on “Saturday Night Live” and in films like “This Is Spinal Tap,” has some of the most extensive extracurricular credits of the “Simpsons” cast. He is the host of the radio program “Le Show,” which offers his weekly perspectives on politics and current events, and starred in the series “Nixon’s the One,” in which he played President Richard M. Nixon in a recreation of his secret Oval Office tapes.

Mr. Shearer was among the “Simpsons” cast members who took a pay cut in 2011 amid tense negotiations to extend the show for its 24th and 25th seasons. In an essay published at that time by The Daily Beast, Mr. Shearer wrote: “For many years now, the cast of ‘The Simpsons’ has been trying to get Fox to agree that, like so many other people who’ve contributed significantly to the show’s success, we be allowed a tiny share of the billions of dollars in profits the show has earned.”

“Instead,” he said, “it’s paid us salaries that, while ridiculous by any normal standard, pale in comparison to what the show’s profit participants have been taking home.”

The show previously retired the character of the schoolteacher Edna Krabappel when Marcia Wallace, the actor who provided her voice, died in 2013. However, Mr. Jean said “The Simpsons” would continue to use characters that Mr. Shearer played. “We do not plan to kill off characters like Burns and Flanders but will recast with the finest voiceover talent available.”