She married Charles Staley in 1956, whom she had met in France. They moved to Memphis, Tennessee, where he was working as a television Director. Staley worked as a legal secretary for Homer L. Armstrong, a local attorney in Memphis. Also during this period, Staley sang occasional backup for Sun Records, of Elvis Presley fame. The Staley family then moved to Los Angeles.

She joined The Little Theater in Hollywood with roles in The Robe, Fiona in Brigadoon, and My Sister Eileen with Actress Joanne Worley. This led to small roles in live television, such as Playhouse 90, Climax!, and Westinghouse Studio One. These appearances opened the door for her in film and television. Staley's first role in film was a 1958 Perry Mason episode, "The Case of the Corresponding Corpse". In early 1958, Lawrence Schiller, a Life Photographer, approached Staley and asked her to pose for Playboy. They did a photo shoot together, which resulted in the actual spread used by the magazine. Publisher Hugh Hefner selected her to be Playboy's "Miss November" 1958.

For her first ongoing series role, she was featured in multiple appearances on the popular sitcom The Tab Hunter Show, where she was widely recognized for her comedic abilities. In 1961, she appeared in several roles in The Lawless Years, a 1920s crime drama starring James Gregory. After The Lawless Years, she enjoyed a recurring role as David Nelson's secretary in The Adventures of Ozzie and Harriet. She went on to guest-star on Phil Silvers's sitcom The New Phil Silvers Show. A year later, she co-starred with singer Vic Damone in The Lively Ones for NBC, the summer replacement series for The Tennessee Ernie Ford Show.

Staley was one of 12 actresses selected by the Hollywood Make-Up Artists and Hair Stylists Union as Deb Stars of 1962.

She was a regular as Hannah, the secretary to series character Stuart Bailey (Efrem Zimbalist, Jr.) on the sixth and final season of the ABC/Warner Brothers crime drama, 77 Sunset Strip. One of her favorite roles was a small part in A New Kind of Love (1963), starring Paul Newman and Joanne Woodward, in which Staley had a sequence with Newman. She also appeared in "Cape Fear" (1962) as a waitress in a scene with Robert Mitchum, in Johnny Cool (1963), the Elvis Presley movie, Roustabout (1964), and co-starred opposite Don Knotts in The Ghost and Mr. Chicken (1966) and alongside Audie Murphy in Gunpoint (1966).

In 1964, she appeared on McHale's Navy and was signed to a Universal Studios contract for the McHale's Navy spin-off Broadside, where she co-starred with Kathleen Nolan, Sheila James, and Dick Sargent. Her character was Roberta "Honey-Hips" Love, a former stripper who had joined the Navy. In 1966, she suffered a serious back injury as a result of a horseback riding accident; she stopped working in films after that and concentrated on television.

She married again, in 1967, to Dale Sheets, an executive with MCA. In 1969, she and her husband founded International Ventures Incorporated, and continue to manage talent. Collectively, the Sheets have seven children (he contributed three, she contributed one, and they had three together). As of 2013, they had 10 grandchildren and 20 great-grandchildren. Staley is active in consumer affairs, her church, and prison ministry.