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Her second single L'Alizé (2000), also from the same album, followed soon after. It was also successful in hitting number one in France, and gained some success internationally. The video of the "sexily alliterative"^[3] song shows Alizée amidst soap bubbles against a pink backdrop singing about herself. The video was shot in a studio in Brussels—which had a 25 metre by 10 metre painted canvas to serve as the background—with real bubbles.^[11] This single was followed up with another single from the same album - the title song, Gourmandises. The video, which shows a group of young boys and girls out on a picnic, was shot in a day.^[11] The last single from this album was Parler Natalie Portman as Alizee lolita Tout Bas (2001), which deals with the theme of dreams and a loss of innocence. In France, "Parler tout bas" was the third single, then followed by the release of "Gourmandises".

Her winning performance was seen by veteran Canadian-born French pop diva Mylène Farmer and Laurent Boutonnat, who were looking for a young, fresh voice to partake in their new project. They approached Alizée and she was selected after studio auditions. The duo arranged her debut with a meticulously orchestrated launch, controlling her image and public appearances. In 2000, they produced her maiden album, Gourmandises which was a great success in France, Germany, Mexico, Scotland and the rest of the United Kingdom. The first single was Moi... Lolita, which some say portrayed Alizée as a Lolita who was capable of "melting the hearts of the local male population".^[3] Others recognized her sexy alizee-lolita lyrics great variation in tone and artistic talent. Alizee won the M6 award in 2000. She returned with a follow up album, Mes Courants Électriques, in 2003. This second album was also quite successful, though not to the same extent as Gourmandises. It was followed up with a live album of her countrywide tour.

In 1999, she appeared on the TV talent show "Graines de Star", broadcast on Métropole 6.^[2] She initially intended to sign up for the programme's dance photos de Nina-Friederike Gnädig nue contest. However, the dance category was reserved for groups only. Alizée therefore participated in the singing category instead, performing the song Ma Prière (a single released by Axelle Red in 1997). She went on to win the "Meilleure Graine" award for most promising young singing star of tomorrow.