The actress passed away on Sunday in Englewood, New Jersey, reported New York Times.
The Broadway star was born in Lynn, Massachusetts to Luther Nichols and Eola Willard in 1934. She attended Stephens College in Columbia before making her stage debut in "Jonah and the Whale" with the Neighborhood Playhouse in 1955.
She won her first Tony award for Best Actress in a Musical in 1961 for the titular character in Meredith Wilson's musical "The Unsinkable Molly Brown."
The award-winning actress went on to star in a multitude of Broadway productions, such as "Rattle of a Simple Man," "High Spirits" and "The Only Game in Town." Grimes won her second Tony Award for 1969's revival of Noel Coward's "Private Lives."
Grimes is survived by her brother and daughter, Tony-winning actress Amanda Plummer.