After two years in college, Gould enlisted in the United States Army during World War II and saw combat in France in a chemical mortar battalion.

[2] After the war, Gould returned to Albany Teachers College and changed his major to study drama and theatre and graduated with a Bachelor of Arts degree in 1947.

Gould began appearing regularly in television in the 1960s and 1970s including roles in the children's sitcom Dennis the Menace, followed by numerous other shows of various types / genres such as – Dr. Kildare, Hazel, The Twilight Zone, The Donna Reed Show, Get Smart, Hogan's Heroes, Gunsmoke, I Dream of Jeannie, The F.B.I., The Big Valley, Mission: Impossible, The Man from U.N.C.L.E., Cannon, and Hawaii Five-O where he made multiple appearances as Honore Vashon, one of that series' most memorable villains.

Midway through the that play's run, after learning the TV series was ready to begin shooting, he decided to honor his commitment to the stage production and passed on the role.

He was "Engulf," the villainous head of a conglomerate, in Silent Movie (1976), directed by Mel Brooks, and made guest appearances on television shows such as Petrocelli, The Love Boat and Soap where he played the hospital roommate of Jody Dallas (Billy Crystal).

Other roles included a married man having an affair with another member of his Yiddish-speaking club in an episode of the PBS series The Sunset Years and as the owner of a deli grooming two African-American men to inherit his business in Singer & Sons.

He portrayed the father of a villain called The Prankster on Lois & Clark: The New Adventures of Superman and made guest appearances on television series such as Felicity, The King of Queens, Touched by an Angel, and Judging Amy.

Gould's film roles in the 1990s and 2000s include appearances in Stuart Little, Patch Adams, The Master of Disguise, the 2003 remake of Freaky Friday, Nobody's Perfect, and Whisper of the Heart.

His stage credits include Broadway theatre plays such as Jules Feiffer's Grown Ups, Neil Simon's Fools, Richard Baer's Mixed Emotions, and Tom Stoppard's Artist Descending a Staircase.

Gould won an Obie Award in 1969 for his work in The Increased Difficulty of Concentration, written by Václav Havel, and reprised the role for a 1988 PBS version of the play.