Born Carolyn Sue Jones in Amarillo, Texas, Jones joined the Pasadena Playhouse in 1947. She secured a contract with Paramount Studios and made her first film in 1952.

In 1953, she married aspiring filmmaker Aaron Spelling (and converted to Judaism upon marriage), and her film career began to gain momentum. A role in House of Wax (1953) brought her good reviews, and she was cast in From Here to Eternity (also 1953), but illness forced her withdrawal. Donna Reed was cast in her role.

She appeared in Invasion of the Body Snatchers (1957), and received a nomination for an Academy Award for Best Supporting Actress for The Bachelor Party (1957). In 1958 she shared a Golden Globe Award for "Most Promising Newcomer" with Sandra Dee and Diane Varsi, and appeared with Elvis Presley in King Creole.

By 1963, she and Spelling were separated, and by 1964 they were divorced. In 1964 she began playing Morticia Addams in the television series The Addams Family, a role which brought her success as a comedian and a Golden Globe Award nomination.

Her acting career began to decline after the end of The Addams Family in 1966, and while she continued to act, her roles were sporadic. While appearing in the television series Capitol in 1982, she was diagnosed with colon cancer and she played many of her scenes in a wheelchair.

Chemotherapy did little to slow the course of the disease and she died the following year at her home in West Hollywood, California at the age of 53 (she had married long-time boyfriend, actor Peter Bailey-Britton, a month earlier).

Carolyn told her sister, Bette Moriarty, that she wanted her epitaph to be, "She gave joy to the world".

She was entombed at Melrose Abbey Memorial Park Cemetery in Anaheim, California.