Carly is a British classically trained singer who has performed in concerts and for corporate events. 

While in Malaysia, she was spotted by the Geneva watchmaker Bedat & Co. In 2014, she was appointed as brand ambassador for the company and, as a direct result, appeared at the David Foster Foundation Miracle Gala.

In November 2014, Paoli made history as the first artist to perform at the International Women's Media Foundation (IWMF) Awards in Los Angeles, hosted by Hollywood actresses Olivia Wilde and Kate Hudson.

In June 2015, Paoli sang a duet with José Carreras in a unique performance at Windsor Castle, for the Prince of Wales

Paoli's song, "Ave Maria", composed by Romano Musumarra with lyrics by Grant Black, was played on Vatican radio as the theme for Pope Francis' Jubilee Year of Mercy in 2016.

In July 2016, Paoli was the headline singer in Music for Mercy, a concert staged in the historic, Roman Forum.

In June 2017, Paoli released her debut album, Singing My Dreams.

In September 2021 released the album Carly Paoli and Friends.