At the age of 14, Charli began recording her debut album, funded by her parents. Two singles, double A-side "Emelline"/"Art Bitch" and "!Franchesckaar!", were released in late 2008 under Orgy Music. Both of these appeared on the record, with versions recorded, along with thirteen other tracks, in 2006.

The album was never commercially released, but Charli did distribute it as a young teenager to her friends at school, as well as selling it at her early shows. In an interview with Idol Magazine, Charli revealed that she wanted her stage name to stand for "Xrated Cunt Xrated",but the label would not allow this.

In 2011, she featured on two singles, "End of the World" by Alex Metric, and "Lost in Space" by Starkey. In May 2011, she released her first single in nearly three years, "Stay Away", followed by "Nuclear Seasons" in November, both produced by Ariel Rechtshaid and released exclusively in the UK.

These singles gained attention from Pitchfork Media, where she gained Best New Track accolades for both tracks, with the former being ranked #35 on their Best Tracks of 2011 list. In late 2011, a five-track promotional sampler of Charli's debut album surfaced. All tracks were early demos, including an early version of "You're the One", titled "In the Dark"

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