Robbie has been acting professionally since 2007, when she starred in two feature films, I.C.U. and Vigilante, both directed by Aash Aaron. After impressing the director with her performance during an audition, she won the lead in I.C.U. without an agent at the time. She has also acted in commercials and featured in a guest role in City Homicide as Caitlin Brentford in 2008.
Robbie began appearing as Donna Freedman on Neighbours from June 2008. The character was originally only a guest role, but she was soon promoted to a regular cast member. In an interview with Digital Spy, Robbie said she had gone on a snowboarding holiday to Canada with her boyfriend soon after auditioning, but had to return after only two days when told that she had won the role.
In early 2009, Robbie appeared in various Network Ten promotions, featuring an ensemble of popular Australian faces on the network. In July 2009, she filled the "Generation Y" guest spot on the Network Ten show Talkin' 'Bout Your Generation. Robbie also became a Youth Ambassador for missing persons as part of National Youth Week.
In the same year, she was nominated for "Most Popular New Female Talent" at the Australian Logie Awards. She was also nominated for "Favorite Hottie" at the Nickelodeon Kids Choice Awards and was up against her Neighbours co-star Dean Geyer. In September 2010, Robbie announced that she was to leave Neighbours after almost three years to pursue an acting career in Hollywood. Her final scenes aired on 26 January 2011 and in April of that year, Robbie was nominated for "Most Popular Actress" at the Logie Awards.
After arriving in Los Angeles for pilot season, Robbie auditioned for the new series of Charlie's Angels. However, the producers at Sony Pictures Television preferred her for a role in ABC drama series Pan Am. Robbie landed the role of Laura Cameron, a newly trained flight attendant. Pan Am was cancelled after one season due to falling ratings. In May 2012, Fiona Bryne of the Herald Sun reported Robbie had joined the cast of Richard Curtis' romantic comedy, About Time. The following month Digital Spy's Zeba Blay announced Robbie was in talks to appear in Martin Scorsese's The Wolf of Wall Street. Linette Lopez from the Business Insider confirmed Robbie's casting in August.