After making her acting debut in the crime film Blow (2001), Roberts gained recognition for her lead role as Addie Singer on the Nickelodeon television teen sitcom Unfabulous (2004–2007). She released her debut soundtrack album, Unfabulous and More, for the series in 2005. She went on to appear in numerous films including Aquamarine (2006), Nancy Drew (2007), Wild Child (2008), Hotel for Dogs (2009), Valentine's Day (2010), It's Kind of a Funny Story (2010), and The Art of Getting By (2011).
Looking for more mature roles, Roberts had starring roles in the films Lymelife (2008), 4.3.2.1. (2010), Scream 4 (2011), Adult World (2013), We're the Millers (2013), and Gia Coppola's Palo Alto (2013). She has since appeared in The Blackcoat's Daughter (2015), Nerve (2016), Who We Are Now (2017), Paradise Hills (2019), Holidate (2020), and the Marvel superhero film Madame Web (2024). She gained further recognition for her starring roles in multiple seasons of the FX anthology horror series American Horror Story (2013–present) and for the lead role of Chanel Oberlin on the Fox comedy horror series Scream Queens (2015–2016).
She is also the co-founder of the book club Belletrist.
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