More than 20 years passed before Gainsbourg released albums as an adult (5:55, IRM, Stage Whisper and Rest) to commercial and critical success.

[5] Gainsbourg was born at the height of her parents' fame; they had made headlines three years earlier with the sexually explicit song "Je t'aime... moi non plus" and by that point had become notorious for their turbulent relationship and multiple artistic collaborations.

Her maternal grandmother was actress Judy Campbell, and her uncle is screenwriter Andrew Birkin, who directed her in The Cement Garden.

[13][14] Gainsbourg attended École Active Bilingue Jeannine Manuel in Paris and Collège Alpin International Beau Soleil[15] in Switzerland.

Gainsbourg would go on to work with her stepfather in the film The Temptation of Isabelle in 1985 and later in Amoureuse in 1992, which also starred her future partner Yvan Attal.

She stated that her mother had pushed her into acting, believing that she wanted to be an actress and encouraging her to make her motion picture debut playing Catherine Deneuve's daughter in the film Paroles et Musique (1984).

That same year Gainsbourg appeared in the film Charlotte for Ever about a man who develops incestuous desires for his teenage daughter after his wife dies.

[22][2] In 1988, she appeared together with her mother in a set of films Kung Fu Master and the documentary drama Jane B. by Agnes V., both directed by Agnès Varda.

In 1993, Gainsbourg made her English-speaking debut in The Cement Garden, written and directed by her uncle, Andrew Birkin.

[23] Gainsbourg starred in the French/Australian production The Tree, released in 2010, and in Lars von Trier's science fiction disaster film Melancholia.

"[27] In 2014, she starred in Three Hearts and Éric Toledano and Olivier Nakache's film Samba, for which she was nominated for a Lumières Award for Best Actress.

In 2000, Gainsbourg was featured on the Soundwalk Collective with Patti Smith album Peradam on the track "The Four Cardinal Times".

In 2006, Gainsbourg released her second album 5:55 to critical acclaim and commercial success, reaching the top spot on the French charts and achieving platinum status in that country.

Gainsbourg attributed the twenty-year break between her debut album and 5:55 to her father's death and her reluctance to explore a musical career without him.

[35] Gainsbourg's head injury in 2007 influenced the title of the album "IRM", an abbreviation for the French translation of magnetic resonance imaging (MRI).

[40] In 2011, Gainsbourg released the double album Stage Whisper, a collection of unreleased songs from IRM and live tracks.

[41] In 2013, Gainsbourg released a cover version of the song "Hey Joe", recorded with Beck, for the soundtrack of the film Nymphomaniac, in which she was the lead actress.

Her music influenced artists such as Tove Lo, who cited the simplicity and quirky lyrical content of Charlotte's IRM as the main inspiration behind her career in music and said that it "opened a new world" for her as regards sound,[42] and she performed a bilingual cover of "The Maiden's Prayer" in French and English as the opening tune for the Anglo-French crime thriller television serial The Tunnel.

Rest is a portrayal of her feelings after the deaths of her father Serge Gainsbourg and her half-sister Kate Barry, with the theme of alcohol addiction.

[49] Throughout late November 2020, Gainsbourg posted images to social media of her in the recording studio with Irish-Scottish music producer Salvador Navarrete, known better by his stage name Sega Bodega.

Gainsbourg's longtime partner is French-Israeli actor/director Yvan Attal whom she met on the set of the 1991 film Aux yeux du monde.

Attal publicly proposed to Gainsbourg on 19 June 2013, during an awards ceremony when he received the French National Order of Merit.