The preparation, characterization, materials properties, crystallization behavior and biodegradability of a polylactide (PLA)/organically modified layered silicate nanocomposite is described. Wide-angle X-ray diffraction and high-resolution TEM analyses confirmed that intercalated stacked and disordered/exfoliated mica layers coexist in the nanocomposite. The nanocomposite showed improved materials properties and crystallization behavior with a simultaneous improvement in biodegradability as compared to neat PLA.