In 1997, Carla Bruni quit the world of fashion to devote herself to music. She sent her lyrics to Julien Clerc in 1999, based on which he composed seven tracks on his 2000 album Si j'étais elle.

In 2002, her debut album Quelqu'un m'a dit, produced by ex-lover Louis Bertignac, was released in Europe with success in Francophone countries. Three songs from the album appear in Hans Canosa's 2005 American film Conversations with Other Women. The song "Le plus beau du quartier" was used in H&M's Christmas 2006 commercial.

In 2005, she was a guest in Louis Bertignac's return album on the song Les frôleuses which they sang as a duet.

In 2006,Carla Bruni recorded "Those Little Things" an English-language translation of the Serge Gainsbourg song "Ces Petits Riens", for the tribute album Monsieur Gainsbourg Revisited. She participated in the opening ceremony of the 2006 Winter Olympics in a parade paying tribute to the Italian flag.

Her second album, No Promises containing poems by Yeats, Emily Dickinson, Auden, Dorothy Parker, Walter de la Mare, and Christina Rosetti, set to music, was released in January 2007.

Her albums are released by the French independent record label Naïve, which releases artists such as Vinicius Cantuaria and Aline de Lima.

At the end of 2007, Carla Bruni was reported to be in a relationship with French president Nicolas Sarkozy after photographers took pictures of them visiting Disneyland Resort Paris, as well as during a vacation in Luxor, Egypt and Petra, Jordan during the Christmas holidays. During a press conference at the Elysée Palace on January 8, 2008, President Sarkozy confirmed their relationship and hinted at a wedding.

They married on 2 February 2008 at the Élysée Palace in Paris. The marriage is Bruni's first and Sarkozy's third.