Nye died Friday of lung cancer at the couple's home, The New York Times reported Monday.
Nye broke onto the Broadway scene in 1960 with her dry wit and Mississippi drawl that attracted comparisons with Tallulah Bankhead, The Times said.
She was nominated for a Tony Award in 1965 for the musical "Half a Sixpence," but most of her stage career was in regional theater. She performed at the Williamstown Theater Festival in northern Massachusetts from 1955 until the late 1970s with leads in "A Streetcar Named Desire," "The Skin of Our Teeth" and "Nude With Violin."
In later years, she appeared in plays by Ibsen, Chekhov and Tennessee Williams at several theaters in New York and New Jersey.
She was nominated for an Emmy Award in 1980 for her portrayal of Bankhead in the TV movie "The Scarlett O'Hara War." Her film roles included "Creep Show" and "Hello Again" and she played different characters on the CBS soap, "Guiding Light" in the 1980s and 2003.
She is survived by her husband.
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