I first heard of Charlotte Gainsbourg from the movie La Science des rêves (The Science of Sleep). She is the daughter of Jane Birkin (for whom the Hermes "Birkin bag" was created), and is a talented singer-songwriter & actress.
She has that quintessentially Parisian persona, so effortlessly stylish, without ever being obvious about it.
Her third album, IRM (French for MRI), is truly a great album. I love the songs Me and Jane Doe, dandelion, and Heaven can wait. Watch the video for Heaven can wait, featuring Beck, below.