Our exhaustive research on the preparation, characterization, materials properties and biodegradability of polylactide (PLA)/organically modified layered silicate (OMLS) nanocomposites has yielded results for PLA/montmorillonite (MMT) nanocomposites. Natural Na+-MMT modified with octadecyl ammonium cation, is used as an OMLS for nanocomposites preparation. The internal structure of the nanocomposites at the nanometer scale is established using wide-angle X-ray diffraction (WAXD) patterns and transmission electron micrographic (TEM) observations. All nanocomposites show improved material properties and crystallization behavior with a simultaneous improvement in biodegradability than that of neat PLA.