She is best remembered for her leading role as the witch Samantha in the ABC situation comedy Bewitched. This show was a huge success during its eight-year run from 1964 to 1972 and remains popular through syndication and the 2005 movie remake starring Will Ferrell and Nicole Kidman. Montgomery received five Emmy Award and four Golden Globe nominations for her role as Samantha.
Montgomery made her television debut in her father's series Robert Montgomery Presents, and her film debut in 1955 in The Court Martial of Billy Mitchell. Her early career then languished, consisting of supporting roles and appearances in television series.
Montgomery refused to do Samantha's famous nose twitch for fans after Bewitched went off the air, and was reluctant to discuss this role. She spent the remainder of her career pursuing dramatic roles that took her as far away from the good-natured Samantha typecasting as possible. She received Emmy Award nominations for playing a rape victim in A Case of Rape (1974), for her portrayal of the notorious Lizzie Borden in The Legend of Lizzie Borden (1975), and for her role as a strong woman facing hardship in 1820's Ohio in the mini-series The Awakening Land (1978). She also made a chilling villain in the 1985 picture Amos, playing a nurse in a state home who terrorized residents Kirk Douglas and Dorothy McGuire. Her final acting role was the Barmaid in an episode of Batman: The Animated Series entitled "Showdown".
Montgomery died in 1995 at the age of 62, from colorectal cancer, eight weeks after being diagnosed with that disease, and her body was cremated. At the time of her death, the media widely reported that she had ignored the symptoms of her illness until it was too late, as she was caring for Foxworth, who had had hip replacement surgery. Unwilling to die in a hospital and with no hope of recovery, she elected to return to the Beverly Hills home she shared with Foxworth, and died there with him and her children by her side.
- The Court-Martial of Billy Mitchell (1955)
- The Twilight Zone (1961), alongside Charles Bronson.
- Johnny Cool (1963)
- Who's Been Sleeping in My Bed? (1963)
- The Victim (1972)
- Mrs. Sundance (1974)
- A Case of Rape (1974)
- The Legend of Lizzie Borden (1975)
- Act of Violence (1979 movie) TV (1979)
- Belle Starr (1980)
- When the Circus Came to Town (1981)
- The Rules of Marriage (1982)
- Amos (1985)
- Face to Face (1990)