In summer 2011, Diamandis and Swedish recording artist Robyn performed as the opening acts for American recording artist Katy Perry's California Dreams Tour. On 30 September, Diamandis released the track "Radioactive" through the iTunes Store; it peaked at number 25 on the UK Singles Chart.
Diamandis's debut single "Obsessions" was released on 14 February 2009 through Neon Gold Records, while her first extended play The Crown Jewels EP followed on 1 June. That summer, she performed at BBC Radio 1's Big Weekend, the Glastonbury Festival, and the Reading and Leeds Festivals. She also performed at iTunes Live, releasing a second EP in July 2009 of performances from that festival.
After spending one month in New York City, Diamandis announced in February 2013 that she had begun writing material for an upcoming third studio album. The single "Froot" was released on 10 October 2014, her 29th birthday, and announced it as the title track.