In 2008, she had her voiceover debut when she voiced the English version of the character Wilma in the CGI-animated family film The Flight Before Christmas. In 2009, Roberts starred alongside Jake T. Austin in Hotel for Dogs, based on the novel by Lois Duncan. The film premiered in January 2009, and took fifth place in its opening weekend with over $17 million. The film has to-date grossed over $114 million, and received generally mixed reviews from critics. Roberts starred as the lead in the film Wild Child, about a rebellious teen from Malibu, California sent to a boarding school in England. Roberts described her character as "pretty much your typical spoiled-brat Malibu socialite who gets shipped off to a British boarding school." Roberts also appeared in the independent film Lymelife with Alec Baldwin, which was premiered at the 2008 Toronto International Film Festival.  In 2010, Roberts co-starred as Grace in the film Valentine's Day in which her aunt, Julia Roberts also appeared, although they were never together on-screen. She also appeared that year in Twelve and It's Kind of a Funny Story. The following year, she co-starred in the film adaptation of Memoirs of a Teenage Amnesiac. She also starred alongside Freddie Highmore in the romantic comedy The Art of Getting By. In 2011, she played the role of Jill Roberts in the Wes Craven film Scream 4.  In 2013, Roberts co-starred with John Cusack and Evan Peters in Adult World. Roberts played a recent college graduate who works at an adult bookstore to make ends meet. She has said that most of her lines were ad-libbed so her reactions in the film were completely genuine. Her performance was praised by both Andrew O'Hehir of Salon and Stephanie Zacharek of The Village Voice, who praised Roberts' performance as "both breezy and carefully tuned". Roberts appears in a supporting role in Dustin Lance Black's Virginia, which received a limited theatrical release in May 2012 after a two and a half year delay. She next appeared in the 2012 film Celeste and Jesse Forever, parodying pop stars such as Kesha with her performance as Riley Banks, an incurious blonde singer. Roberts said in an interview that her role as Banks tempted her to write an album of songs using her character as an alter ego.

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She next appeared in the 2012 film Celeste and Jesse Forever, parodying pop stars such as Kesha with her performance as Riley Banks,