Buckley began her career in 2008 as a contestant on the BBC TV talent show I'd Do Anything, in which she came second. A RADA graduate, her early onscreen appearances were in BBC television series, such as War & Peace (2016) and Taboo (2017). Buckley made her film debut playing the lead role in Beast (2017) and had her breakthrough starring in the musical film Wild Rose (2018). Her performance as an aspiring country music singer in the latter earned her a nomination for the BAFTA Award for Best Actress in a Leading Role.
Buckley's career progressed with starring roles in the HBO miniseries Chernobyl (2019), I'm Thinking of Ending Things (2020), season four of Fargo (2020), The Lost Daughter (2021), Men (2022) and Women Talking (2022). Her performance in The Lost Daughter earned her nominations for the BAFTA Award for Best Actress in a Supporting Role and the Academy Award for Best Supporting Actress. Buckley's portrayal of Sally Bowles in a 2021 West End theatre revival of Cabaret won her the Laurence Olivier Award for Best Actress in a Musical.
In 2022, she released the collaborative album For All Our Days That Tear the Heart with Bernard Butler, which was shortlisted for the 2022 Mercury Prize.
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