In 2010 she formed Tune in Tokyo, an electro-pop band, with producer Paul Brandoli, they released two singles, "Dreamer" (November 2010) and "Ray of Love" (April 2012).

By August that year Gauci was living and working in London both as a recording artist and music teacher.

[5][8] Gauci performed as a session musician, and in 2002, she began writing her debut three-track extended play, Take It or Leave It,[9] which was released in 2006.

[3] She performed an original song, "Free Falling", co-written by Gauci with James Kempster;[14] and a rendition of Gloria Gaynor's "I Will Survive".

Her performances have earned acclaim; The Courier-Mail noted her renditions of Rihanna's "Umbrella", Kate Bush's "Running Up that Hill", and Gnarls Barkley's "Crazy" as highlights.

[16] Her performances of "Umbrella", Divinyls' "Boys in Town", and Morgan Lewis's "How High the Moon" earned "touchdowns" from Holden.

[25] Unlike Damien Leith's Winners Journey of the previous year, Gauci's CD/DVD did not include Australian Idol stage performances.

[26] This drew criticism with Fremantle Media, producers of Australian Idol, suggesting Gauci's record label, Sony BMG, had deliberately excluded the material.

She took three musicians from the Natalie Gauci Band, as well as a long time keyboard collaborator and music director, while she sang and played the piano.

[34][35] In 2010 Gauci formed Tune in Tokyo, an electro-pop and dance music band, with producer Paul Brandoli.

She told the Daily Telegraph that she had changed her style after hanging out in Melbourne's gay dance clubs with musician, and her then-husband, Hamish Cowan (Cordrazine).

[39] She revealed that she was working on the group's debut album and that she had made a cameo for a 2011 film, Big Mamma's Boy, which stars actress, Holly Valance.

[40] In 2011 Gauci travelled to Europe, where she worked with producers and DJ's, by August 2012 she had moved to London where she continued her recording and teaching music careers.

[43][44] During early 2012 Gauci toured Europe including Spain, Belgium, Italy, The Netherlands and Germany before settling in Sweden.

[45] There she co-wrote a new single, "Just Dance", with local songwriters, Jonas and Jeanette von der Burg, which was issued on Four on the Floor Records in May.

On 20 November an Italian duo of DJ-producers, Jack & Joy (aka Max Bondino and Luca Loi) issued their single, "We Are the Stars" featuring Gauci, on Adaptor Recordings.

[51] In 2020 she was a contestant in the ninth season of The Voice (Australian TV series), with the audition song "The Greatest" and choose team Guy.

[53] On 28 March 2009 Gauci married Hamish Cowan, the lead singer of art rock band, Cordrazine.

[56] Cowan declared "I would love to do a duet with her, she inspires me and is my muse... Nat's passion and unwillingness to compromise her art and vision keeps me focused and betters me in every way.

Gauci had worked as a personal trainer for Australian Idol judge, Ian "Dicko" Dickson during 2009–10.