With the birth of her daughter in 2003 Natalie began Leave Your Sleep / Leave Your Suppper, a seven-year-long project that led to the recording of a double album in 2010 of musical adaptations of classic children’s poetry. Among the poets’ work she selected were British Victorians such as Edward Lear, Christina Rossetti, Robert Louis Stevenson and Gerard Manley Hopkins and 20th century American writers, e.e. Cummings and Ogden Nash, etc. She drew from a wide range of stylistic musical settings to illustrate the poems. She collaborated with 130 different musicians including from Cajun band to early music consort to Chinese music ensemble Wynton Marsalis and Quintet, Medeski, Martin & Wood, The Klezmatics, The Ditty Bops, The Memphis Boys, The Fairfield Four, Hazmat Modine, Lúnasa and members of the New York Philharmonic. The album was produced by Natalie and Andres Levin and with a few exceptions all the sessions were engineered by Nick Wollage, assisted by Eli Walker at the Clubhouse in Rhinebeck, NY.

Leave Your Sleep included a handsome 80-page hardcover book (by award winning British book designer David Pearson) with biographical essays on the poets by Natalie and archival portraits obtained from libraries, museums and private collections in both the US and UK. This was the first of several albums to be released by Nonesuch Records. In 2012 Leave Your Sleep was the inspiration for a beautiful children’s book illustrated by Barbara McClintock through MacMillan Publishing.