Segal, who was Oscar-nominated for 1966 black comedy-drama ‘Who's Afraid of Virginia Woolf?’, died on Tuesday in Santa Rosa, California.
Sonia Segal, his wife said: "The family is devastated to announce that this morning George Segal passed away due to complications from bypass surgery."
Since 2013 Segal, also a skilled banjo player, had played Albert 'Pops' Solomon on TV comedy ‘The Goldbergs’.
He starred as magazine publisher Jack Gallo in the US sitcom ‘Just Shoot Me’ from 1997 to 2003.
Segal's portrayal of Nick in the Mike Nichols-directed ‘Who's Afraid Of Virginia Woolf?’ earned him a best supporting actor nomination at the Oscars.
His co-stars - Richard Burton, Elizabeth Taylor and Sandy Dennis - were also nominated, with both women winning.
Wendi McLendon-Covey, Segal's The Goldbergs co-star, was among those to pay tribute online.
Alongside a picture of her with the late actor, she wrote: "Grateful."
The Goldbergs creator, Adam F Goldberg, described Segal as a "legend".
He said: "It was a true honour being a small part of George Segal's amazing legacy. By pure fate, I ended up casting the perfect person to play Pops.
"Just like my grandfather, George was a kid at heart with a magical spark."
Melissa Joan Hart, star of Sabrina The Teenage Witch who directed Segal in an episode of The Goldbergs.
In her tribute, she said: "Shocked and saddened to hear of #GeorgeSegal passing away!
"He was a true gem and great man. He will be missed!"
Segal also starred in films Bye Bye Braverman, A Touch Of Class, The Hot Rock and Fun With Dick And Jane.
He was honoured with a star on the Hollywood Walk Of Fame in 2017.
It is understood Segal's last episode on The Goldbergs will be broadcast in early April.
A spokesman for ABC Entertainment said: "For eight years, George Segal made us laugh as Pops on The Goldbergs, but his legacy in the entertainment world spans decades.
"His talent has left an indelible mark and we're grateful for the laughter and joy he has given us all.
"Our thoughts and deepest condolences are with his wife, Sonia, and his family during this difficult time."