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Hartley has made appearances in many British productions, including films such as Northern Soul and Me and Her both in 2004; Terra Firma and Flushed in 2008; and The Crossing, Janet and Bernard and I Don't Care in 2014. Hartley has been a character actor in many TV films and TV series since 2004, with her most notable roles in This Is England '86, This Is England '88 and This Is England '90, the follow-on TV mini-series to the film. In movies Hartley has appeared in This Is England (2006) as Cynthia,and the feature film The Young Victoria in 2009, with Emily Blunt and Rupert Friend.
In 2016 Hartley appeared as Janette, Eddie's mother in the film Eddie the Eagle appearing alongside Taron Egerton and Hugh Jackman.She co-starred in the David Cross series Bliss opposite Heather Graham as one of two partners of a fraudulent travel writer.Hartley also appeared in the comedy horror film Slaughterhouse Rulez, alongside Asa Butterfield and Simon Pegg.
After a successful pilot episode, Hartley played the role of Bethan's mum `Katrina' who suffers from bipolar disorder in the BBC series In My Skin which aired on BBC1 in 2020.In April 2020, Hartley returned as June in the second series of Ricky Gervais's After Life.
In January 2021, Hartley joined the Rising Star Award jury of the EE British Academy Film Awards to select the shortlist for the 2021 award, alongside Alicia Vikander, Naomi Ackie and several other prominent figures of the industry.In September 2021, Hartley plays the lead character in the upcoming British comedy film Swede Caroline, the first for Deadbeat Studios. In November 2021, Hartley was nominated for the BIFA Award for Best Supporting Actress for her performance as Tina in the Marley Morrison directed British drama film Sweetheart.
In December 2021, Hartley had a guest-role appearance in the BBC TV special — We Wish You A Mandy Christmas alongside Diane Morgan and Johnny Vegas.