This chapter aims at exploring the revolutionary field of nanotechnology and some of its promising aspects in polymer nanocomposites in view of preparation, characterization, materials properties, and processing of polymer layered silicate nanocomposites. These materials are attracting considerable interest in polymer science research. Polymer layered silicate nanocomposites are an important class of hybrid, organic/inorganic materials with substantially improved mechanical, thermal, and thermomechanical properties in comparison to pristine polymers. In addition, they also show superior ultraviolet (UV) as well as chemical resistance and are widely being investigated for improving gas barrier and flame retardant properties. Hectorite and montmorillonite are among the most commonly used smectite-type layered silicates for the preparation of polymer-clay nanocomposites. Smectites are a valuable mineral class for industrial applications due to their high cation exchange capacities, surface area, surface reactivity, adsorptive properties, and, in the case of hectorite, high viscosity and transparency in solution. A wide range of polymer matrices are explored for the preparation of polymer-clay nanocomposites, however, this chapter deals with special emphasis on biodegradable polymers--cellulose and natural rubber. Also, the chapter describes the common synthetic techniques in producing polymeric layered silicate nanocomposites, its properties, and applications.