The North Carolina native, who originated the role of Nick in the 1962 play, "Who's Afraid of Virginia Woolf?," played Hamlet, Henry V, President John Adams and Big Daddy in a career that spanned more than five decades, the Los Angeles Times said.
Grizzard won a Tony Award in 1996 for his performance as Tobias in a revival of Edward Albee's "A Delicate Balance."
Among his film credits are "Advise & Consent" and "Comes a Horseman" and he earned an Emmy Award in 1980 for his work in "The Oldest Living Graduate."
"What was remarkable about his acting was he didn't seem to be acting at all," said Andre Bishop, artistic director of New York's Lincoln Center Theater. "There was no sense of effort or strain ... The curtain went up and there was George, just being this character."