She was also a singer in the indie pop group the Pipettes, whose debut We Are the Pipettes was described by Pitchfork as "a classic modern indie-pop album".
From the age of five she attended the Seán Éireann-McMahon Academy of Irish Dance and was a cast member of Michael Flatley's productions of Lord of the Dance and Feet of Flames by the age of 17, playing a lead role in a Las Vegas production of the former. In 2001 she had a role in the Welsh language soap opera Pobol y Cwm on S4C, for whom she would later host her own programme Ydy Gwenno'n Gallu...? She is fluent in Welsh language and Cornish language. On 18 April 2019 she presented "Songs from the Edgelands", a programme about songs in minority languages on BBC Radio 4. Radio Times; 13–19 April 2019
In June 2012, Saunders released a five-song Welsh language EP, Ymbelydredd, available on hand-painted cassettes on Peski Records.
Gwenno appears on The Boy Least Likely To's 2013 album The Great Perhaps, contributing vocals to the track "It Could've Been Me".
She released her first solo full-length album, the Welsh-language Y Dydd Olaf, in October 2014 on Peski Records. This album was inspired in part by the dystopian science fiction book of the same name by Owain Owain. In May 2015, Gwenno was signed to Heavenly Recordings. The label re-released her debut album in July. The album won Best Welsh Album at the 2015 National Eisteddfod and in November 2015 won the 2014–2015 Welsh Music Prize.
Gwenno also co-produced and co-hosted a Welsh radio show on Cardiff Radio titled "Cam O'r Tywyllwch" ("A Step Away from the Darkness") with her Peski Records colleagues. The team was also behind the CAM '15 music festival in Cardiff, which took place in April 2015 and featured the first live performance in over 20 years by Welsh music post-punk pioneers Datblygu.
She released her second solo album Le Kov in 2018, which was an all-Cornish language album. It centred on themes of "the struggle of Kernewek the and the concerns of Cornish cultural visibility as the perceptions of a timeless and haunted landscape often clash with the reality of intense poverty and an economy devastated by the demands of tourism". The album saw Gwenno touring and headlining in Europe and Australia, and supporting acts such as Suede and the Manic Street Preachers, with whom she re-recorded a verse of the song "Spectators of Suicide" in Welsh, as well as singing on an English version of the song with the band. A successful performance of "Tir Ha Mor" on Later... with Jools Holland prompted wider conversations on the state of the Cornish language with Michael Portillo, Jon Snow, and Nina Nannar. Le Kov was named one of the best albums of 2018 by The Guardian, Uncut and Mojo.
Her third solo album Tresor, also a Cornish language album, releases on 1 July 2022 on Heavenly Recordings. It is inspired by powerful woman writers and artists such as Ithell Colquhoun, the Cornish language poet Phoebe Proctor, Maya Deren and Monica Sjöö, Tresor is an intimate view of the feminine interior experience, of domesticity and desire, a rare glimmer of life lived in and expressed through Cornish. On 26 July, Tresor became Gwenno's first album to be nominated for the Mercury Prize, and it was named one of the albums of the year by BBC Radio 6 Music.
On 7 April 2025, Gwenno announced her fourth solo album, Utopia, set for release on 11 July by Heavenly. The lead single, "Dancing on Volcanoes", was released with the announcement. The album is her first primarily in the English language.
In October 2018, the Cornish Language Board claimed that Saunders's album Le Kov had contributed to a 15% increase in the number of people taking Cornish language exams during 2018.
Wales Arts Review included two of Gwenno's albums on their 2021 list of the greatest Welsh albums of all-time: Le Kov at 18 and Y Dydd Olaf at 64.
Saunders is a supporter of Welsh independence. She has said: "What if there are other ways of co-existing? What if we can organise ourselves differently? There is an innate anarchy to art and an absolute potential in utilising it for the good whilst imagining better futures. We want to continue a conversation about an inclusive self-determination by drawing on our past, embracing our neighbours across the UK and the world with open arms, whilst also making sure that we're singing along to the best possible tune". She was made a Gorsedh Kernow in 2019 for "services to the Cornish language through music and the media".
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