From October 2009 to January 2010 Vickers played the title role in a West End revival of The Rise and Fall of Little Voice for which she won the award for "London Newcomer of the Year" at the Theatregoers' Choice Awards. Vickers' debut single, "Once", charted at number one on the UK Singles Chart after its release on 19 April 2010 and has sold over 210,000 copies in the United Kingdom. Vickers' debut album was released on 3 May 2010 in the United Kingdom achieving number one status on the UK Albums Chart, number seven on the Irish Albums Chart and number four on the European Top 100 Albums, and has been certified Gold by the BPI. Songs from the Tainted Cherry Tree went on to sell over 200,000 copies in the United Kingdom.
Her second single, "The Boy Who Murdered Love", charted at number 36 on the UK Singles Chart. This was followed by her third single, "My Wicked Heart", which was released on 17 October 2010 digitally and on 1 November 2010 physically. "My Wicked Heart" peaked at number 13 on the UK Singles Chart, making it Vickers' third consecutive Top 40 single.