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Cruz made her television acting debut at age 16, and her feature film debut the following year in Jamón Jamón (1992). Her subsequent roles included Belle Époque (1992), Open Your Eyes (1997), Don Juan (1998), The Hi-Lo Country (1999), The Girl of Your Dreams (2000) and Woman on Top (2000). She collaborated with Spanish director Pedro Almodóvar in Live Flesh (1997), All About My Mother (1999), Volver (2006), Broken Embraces (2009), I'm So Excited! (2013), Pain and Glory (2019), and Parallel Mothers (2021).

For her role in Woody Allen's romantic drama Vicky Cristina Barcelona (2008), Cruz won the Academy Award for Best Supporting Actress. Her other Oscar-nominated roles are in Volver (2006), Nine(2009), and Parallel Mothers (2021). Other films include Vanilla Sky (2001), Blow (2001), Pirates of the Caribbean: On Stranger Tides (2011), The Counselor (2013), Murder on the Orient Express (2017), Everybody Knows (2018), Official Competition (2022), L'immensità (2022), and Ferrari (2023). For her role as Donatella Versace in the miniseries The Assassination of Gianni Versace: American Crime Story (2018), she received a Primetime Emmy Award nomination. She is the only Spanish actress to have won an Academy Award and to have received a star on the Hollywood Walk of Fame. In 2007, she won the David di Donatello for the leading role in Don't Move.

Cruz has also modelled for Mango, Ralph Lauren, and L'Oréal, and has designed clothing for Mango with her younger sister, Mónica Cruz. She has been a house ambassador for Chanel since 2018. She volunteered in Uganda and India, where she spent one week working with Mother Teresa, and donated her salary from The Hi-Lo Country to help fund the now-deceased nun's mission.