Wallace, who earlier played the quick-witted receptionist on 'The Bob Newhart Show', died following a long battle with an unspecified illness at her home in Los Angeles, surrounded by her family, reported TMZ online.
"I was tremendously saddened to learn this morning of the passing of the brilliant and gracious Marcia Wallace. She was beloved by all at The Simpsons and we intend to retire her irreplaceable character," said Al Jean, 'The Simpsons' executive producer, in a statement.
"Cheers to the hilarious, kind, fab Marcia Wallace, who has taken her leave of us. Heaven is now a much funnier place because of you, Marcia," Yeardley Smith, who voices Lisa Simpson, wrote on Twitter.
That was her 10th of 177 episodes on the series.
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On 'Newhart', which aired on CBS from 1972 to 1978, Wallace played Carol Kester, the wise-cracking, independent receptionist in a Chicago high rise that housed the offices of psychologist Bob Hartley (Newhart) and orthodontist Jerry Robinson (Peter Bonerz).
She was in 139 of the show's 142 episodes.
In addition to her well-known role on 'The Simpsons' and 'The Bob Newhart Show' throughout the 1970's, she also featured on shows as 'Bewitched', 'The Brady Bunch', 'Murder She Wrote' and 'Full House'.