I can't compose music or write lyrics, and I'm not a trained musician," says French actor and singer Charlotte Gainsbourg, smoking a cigarette at Hollywood's Sunset Sound studios. "The evolution of making an album is a mystery." But when you're the daughter of French cultural icon Serge Gainsbourg and actress Jane Birkin – and the star of films by Michel Gondry and Lars von Trier — getting international cool hunters to help you translate your certain je ne sais quoi into an album of 13 songs is about as easy as lighting a smoke. For her 2006 set, 5:55, the 38-year-old worked with Jarvis Cocker and Air; on the upcoming IRM (the title is French for "MRI"; Gainsbourg suffered a brain aneurysm in 2007), she roped in Beck, who produced, co-wrote and performed on the entire record. "Without really talking about it, things just happened," she says. "By the time we went into the studio, he'd prepared tons of stuff." Must be nice.
Recording in L.A. during breaks between films (hers) and albums (his), the two crafted a disc that casually mixes French and Englis, and leaps between elegant, atmospheric pop ("Le Chat du Café des Artistes") and sleazy blues rock ("Trick Pony") Beck counts Captain Beefheart and proto-country singer Jimmie Rodgers as big influences on the LP. "In my world, the 1930 still feels contemporary," he says. "That feels more current and valid to me than new music." As for Gainsbourg's singing – breathy, ethereal, half-sung, half-spoken – it's not something she needs to think about. I always go back to my father," she says. "It's just something I do."
This story is from the January 21st, 2010 issue of Rolling Stone.