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Burstyn made her acting debut on Broadway in Fair Game in 1957 before winning the Tony Award for Best Actress in a Play for Same Time, Next Year (1975). She earned the Academy Award for Best Actress as the widow Alice Hyatt in Martin Scorsese's romantic drama Alice Doesn't Live Here Anymore (1974). Her other Oscar-nominated roles were in The Last Picture Show (1971), The Exorcist (1973), Same Time, Next Year (1978), Resurrection (1980), and Requiem for a Dream (2000). Her other notable films include Harry and Tonto (1974), How to Make an American Quilt (1995), Divine Secrets of the Ya-Ya Sisterhood (2002), W. (2008), Interstellar (2014), The Age of Adaline (2015), and Pieces of a Woman (2020).

She won Primetime Emmy Awards for her guest role in the NBC legal drama Law & Order: Special Victims Unit (2009) and supporting role in the USA Network political miniseries Political Animals (2013). Her other Emmy-nominated roles include Pack of Lies (1988), Mrs. Harris (2005), Big Love (2008), Draft Day, Flowers in the Attic (both 2014), and House of Cards (2016). Since 2000, she has been co-president of the Actors Studio, a drama school in New York City. In 2013, she was inducted into the American Theatre Hall of Fame for her work onstage.