The singer (26) has signed up to perform at the V Festival, which will be headlined by rockers Kings Of Leon and Kasabian.
Girls Aloud played at V, a weekend event at Hylands Park in Chelmsford and Weston Park, Staffordshire, two years ago.
X Factor judge Cole announced last week that she and husband Ashley Cole were splitting up following reports that the England and Chelsea football star had been repeatedly unfaithful.
Performers at the 15th anniversary festival, which takes place on August 21 and 22, will also include Florence And The Machine, Stereophonics and Faithless.
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