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Murray's first television role was in Skins, playing the role of Cassie Ainsworth, a gentle, "spacey", yet self-destructive teenager with an eating disorder. At nearly 17 years old, she had learned that auditions were taking place for the series through her local youth theatre and decided to audition for the experience. She and April Pearson were the first two to get cast for the show. Murray went on to appear in the first two series which broadcast in 2007–2008 on E4. Along with the primary cast members, she left at the end of the show's second series to make way for a new generation of characters. On the decision to replace the cast, Murray has said that "it would be really silly to be in a teenage drama if you're no longer a teenager"
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Garai enjoys travelling and cooking in her spare time, calling it 'therapeutic' in many ways. She has visited Hong Kong, Malaysia, Italy, Austria, Morocco, Switzerland and the United States, "To be the outsider for a period of time changes you for the better. It shakes up your comfort level. You have to really make an effort to enter into other people's culture and psychology and language, which the British are very bad at doing."
She is currently expecting her first child with her boyfriend, British actor Sam Hoare
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