In 2010, Gillies was cast as bad girl and occasional antagonist Jade West in the Nickelodeon television show Victorious, a sitcom revolving around teenagers at a performing arts-based high school in Hollywood. This marked her second time working alongside 13 co-star Ariana Grande. The show premiered on March 27, 2010. During her time on Victorious, Gillies was featured in several songs on the soundtracks Victorious and Victorious 2.0, including "Give It Up" (duet with Ariana Grande), and "Take a Hint" (duet with Victoria Justice). She also wrote and recorded the song "You Don't Know Me" for an episode of Victorious, and it was later featured in Victorious 3.0. She lent her talents to other Nickelodeon shows, voicing the character of Daphne on the animated series Winx Club and recording Winx Club's official song, "We Are Believix." She also appeared in an episode of Big Time Rush and as a contestant on game shows BrainSurge and Figure It Out.
Beginning in 2012, Gillies began playing small guest roles outside of Nickelodeon. Notable appearances include White Collar and The Exes. In July 2012, it was reported that Gillies was working on an alternative rock album. Victorious ended on February 2, 2013 after four seasons. Following the cancellation of the series, Gillies took some time off from acting. In 2013, she was cast as Courtney in the musical adaptation of Jawbreaker and participated in a reading of the show in Manhattan. The musical did not end up being taken to Broadway. On December 10, 2013, Gillies recorded a duet with Ariana Grande called "Santa Baby" for Grande's Christmas EP Christmas Kisses. In 2014, Gillies appeared in the horror film Animal as Mandy, which was filmed in the summer of 2013 in Manchester, Connecticut and was produced by Drew Barrymore. The film also features Gillies' former Winx Club co-star Keke Palmer and was released on iTunes June 17, 2014. Gillies reprised her role as Jade in a special episode of the iCarly and Victorious spinoff series Sam and Cat. Killing Daddy, a Lifetime original movie, stars Gillies as Calista "Callie" Ross, a troubled young woman who returns to her estranged family with a plan for her recently disabled father and her inheritance. The movie aired on Lifetime on July 5, 2014.
In 2015, Gillies was cast as Heather in the remake of Vacation. The film received a wide release on July 29, 2015. She was then cast in the comedy series Sex&Drugs&Rock&Roll as Gigi, an aspiring singer and daughter of a former rock star named Johnny Rock (portrayed by the show's creator Denis Leary). The show premiered July 16, 2015 to mixed reviews, but Gillies' performance as Gigi was well-received. The show ran for two seasons, with the second season finale airing on September 1, 2016. On September 9, 2016, FX declined to renew the show for a third season, effectively canceling the series.
In February 2017, Gillies was cast in the role of Fallon Carrington in The CW's Dynasty reboot.
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