Gould was born in Brooklyn, New York. His mother, Lucille (née Raver), sold artificial flowers to beauty shops, and his father, Bernard Goldstein, worked in the garment business as a textiles buyer. His family was Jewish, and his grandparents were immigrants from Ukraine, Poland, and Russia. He graduated from the Professional Children's School.
Gould began acting in the Broadway theatre in the late 1950s, making his Broadway debut in Rumple (1957). He was in Say Darling (1958-59) and had a number of small parts in the successful musical Irma La Douce (1960-61), Say, Darling.
Gould had a starring role in I Can Get It for You Wholesale (where he met Barbra Streisand) in 1962, which went for 300 performances. Other roles included Drat! The Cat! (1965), and Little Murders (1967).
Gould made his film debut in Quick, Let's Get Married (1966). His first notable movie role was in The Night They Raided Minsky's (1968), directed by William Friedkin.
Gould leapt to international fame playing one of the four leads in Bob & Carol & Ted & Alice (1969), which was a huge hit. He earned a nomination for the Academy Award for Best Supporting Actor.
Gould followed it playing Trapper John in Robert Altman's satirical 1970 film MASH. It was another success.
Gould's third film as star was Getting Straight (1970) where he played a Vietnam veteran who gets involved in student protests. Not as popular as the other two movies, it was still a success and Gould was now one of the biggest stars in the country. Time magazine placed him on one of its covers in 1970, calling him a "star for an uptight age".
Gould went into a comedy, Move (1970) with Paula Prentiss that was his first flop. Also unsuccessful was I Love My Wife (1970) with Brenda Vaccaro, which he had turned down McCabe and Mrs Miller to do.
Gould had bought the film rights to Little Murders (1971) and produced and starred in the film version, directed by Alan Arkin. It was a commercial disappointment, although it has become a cult favourite.
Gould received an invitation from Ingmar Bergman to appear in Bergman's first English-language film The Touch (1971). It received mixed reviews and failed at the box office.
Gould also bought film rights to the novel A Glimpse of Tiger, and started filming it as part of a two picture deal with Warner Bros. The movie was abandoned during shooting after only four days after rumours that Gould was on drugs.
Gould was unemployed for a year and a half. He and his producing partner helped make Everything You Always Wanted to Know About Sex* (*But Were Afraid to Ask) (1972) and later sold it to United Artists. Gould says he was offered the lead in Pocket Money but turned it down because he did not want to work with Stuart Rosenberg again. Gould eventually mae a comeback in The Long Goodbye (1973).
Gould's career recovered when he received an offer to play detective Philip Marlowe in Altman's 1973 film noir The Long Goodbye. The role had previously been played by such distinguished actors as Humphrey Bogart and Dick Powell, and would later be essayed by Robert Mitchum, but Gould's naturalistic performance represented Altman's modern, somewhat controversial revision of the material. The movie was not a huge hit but has come to be regarded as one of Gould's best films.
Gould says Warner Bros offered in Freebie and the Bean (1974) but he turned it down. Instead he made a science fiction film shot in England, Who? (1974). Better reviewed was California Split (1974) where Gould played a gambling addict alongside George Segal in California Split (1974).
He appeared in two other "buddy" movies: Busting (1974) with Robert Blake for Peter Hyams, and S*P*Y*S (1974) with Sutherland.
Gould had a cameo as himself in the Altman film Nashville (1975), and another cameo in Mean Johnny Barrows (1976). He starred in a comedy, Whiffs (1975) and did a romantic comedy with Diane Keaton, I Will, I Will... for Now (1976). Keaton was also in Harry and Walter Go to New York (1976) with Gould, James Caan and Michael Caine.
He hosted Saturday Night Live six times, his final time being the first episode of the disastrous Jean Doumanian season (season 6) in November 1980, where he was shocked to find that the original cast and producer had left and a new cast and producer had taken their place. He has never hosted after that, but appeared in a season 16 (1990–1991) episode hosted by Tom Hanks where Hanks is welcomed into the Five-Timers club, a society for celebrities who have hosted SNL five times or more.
Gould was one of several stars in A Bridge Too Far (1977) and had the lead in a boxing kangaroo comedy, Matilda (1978).
Gould had his first hit in a while with Capricorn One (1977), directed by Hymans. It was financed by Lew Grade who also invested in The Muppets on which Gould would guest star.
He went to Canada to star in a highly regarded thriller The Silent Partner (1978) then made another for Grade, Escape to Athena (1978). In England he appeared in the much-maligned remake of of The Lady Vanishes (1979). He had a cameo in Grade's The Muppet Movie (1979).
Gould starred in a film with Susannah York, Falling in Love Again (1980) which flopped. He made two films for Disney, The Last Flight of Noah's Ark (1980) and The Devil and Max Devlin (1981).
He was in a comedy Dirty Tricks] (1981) and made Tramps (1983) in Austria. He was in a Broadway flop The Guys in the Truck in 1983.
He supported Roger Moore in The Naked Face (1984) and was the lead in Over the Brooklyn Bridge (1984).
Gould starred in a sitcom called E/R in 1984–1985. He had the lead in Inside Out (1986) and went to Italy for My First Forty Years (1987). On TV he was in Conspiracy: The Trial of the Chicago 8 (1987) and Frog (1988).
After supporting Whoppi Goldberg in The Telephone (1988) he had the lead inDangerous Love (1988) and the Australian mini series Act of Betrayal (1988).
Over time Gould became more of a supporting actor. He could be seen in Night Visitor (1989), The Big Picture (1989), Massacre Play (1989), and The Lemon Sisters (1990). He did play the lead in Dead Men Don't Die (1991).
Gould received critical praise for his performances as an aging mobster in Warren Beatty's 1991 film Bugsy. He cameoed as himself in Altman's The Player (1991) and went to Australia for Exchange Lifeguards (1992).
He had a semi-recurring role as the father of Courteney Cox and David Schwimmer on the sitcom Friends. He played the boyfriend of the protagonist's mother in American History X (1998).
He also co-starred as Reuben Tishkoff in the popular "caper" film Ocean's Eleven (2001) and its sequels: Ocean's Twelve (2004) and Ocean's Thirteen (2007). Other recent films roles include supporting turns in Contagion (2011) and Ruby Sparks (2012).
In 2005 he was the guest star in a feature-length episode of the UK TV series Poirot, The Mystery of the Blue Train, and he has recently guest starred on a number of television series including Law & Order and CSI. He has also loaned his voice to several animated series, most notable among them, the Disney Channel animated series Kim Possible and the 2006 video game Scarface: The World Is Yours.
Gould had a memorable role playing Ezra Goldman on Showtime's Ray Donovan from 2013 to 2016.
Gould currently serves on the Screen Actors Guild National Board of Directors.
Gould has said that he has a "very deep Jewish identity". He has been married three times, twice to the same woman:Barbra Streisand (March 21, 1963 – July 9, 1971; divorced; 1 child, actor Jason Gould)
Jennifer Bogart (December 8, 1973 – 1975; June 9, 1978 – 1979). They were divorced twice. The couple had two children. Jennifer's father was director Paul Bogart.
Gould became one of the many celebrity producers of The 1 Second Film collaboration in June 2009 and is known for his association to charitable causes such as Save Ellis Island.