Gould began acting in films with an uncredited role in T-Men (1947). She appeared in several uncredited roles for the remainder of the decade, and received her first screen credit with The Story of Molly X (1949).
In 1953, Gould appeared as a guest in an episode of Letter to Loretta with Loretta Young. She continued to guest star in the 1950s and 1960s in such television series as I Love Lucy, December Bride, Maverick, The Flintstones, The Twilight Zone, The Lucy Show, Burke's Law, I Dream of Jeannie, Love, American Style , Gilligan's Island and Mister Ed. She played a prominent supporting role in the film The Ghost and Mr. Chicken in 1966.
In 1963 Sandra Gould released a comedy single record entitled: Hello Melvin (This Is Mama) as an 'answer' to Allan Sherman's hit: Hello Muddah, Hello Faddah.
Following the death of actress Alice Pearce in 1966, Gould replaced her as the nosy neighbor Gladys Kravitz on the popular ABC sitcom Bewitched.
After Bewitched ended in 1972, Gould made appearances on TV shows including The Brady Bunch, Adam-12, Punky Brewster, Friends and Veronica's Closet. In 1977, Gould reprised her role as Gladys Kravitz on the unsuccessful Bewitched spin-off series, Tabitha. She also appeared in the movie, "Skatetown U.S.A.," in 1979.
Gould wrote two books, Always Say Maybe and Sexpots and Pans, published by Golden Press. Twice married, she was the widow of broadcasting executive Larry Berns, and had one son, Michael. She died immediately following heart surgery three days before her 83rd birthday.