Segal's wife Sonia Segal confirmed his death in a statement.
"The family is devastated to announce that this morning George Segal passed away due to complications from bypass surgery," she said.
The Hollywood star portrayed family patriarch Albert 'Pops' Solomon on ABC's The Goldbergs since the series started in 2013.
"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," the official Twitter account for The Goldbergs said.
Segal was fashion magazine owner Jack Gallo in Just Shoot Me!, which earned him a Golden Globe award. He won his first Golden Globe for starring in 1973 romantic comedy A Touch of Class.
The actor earned an Oscar nomination for portraying young husband Nick in 1966's Who's Afraid of Virginia Woolf? He also starred in films Ship of Fools, Fun with Dick and Jane, The Duchess and the Dirtwater Fox, Where's Poppa?, Blume in Love, For the Boys and King Rat, among others.