The present invention is directed to processes for preparing a silicone surfactant intercalated clay and a polymer-clay nanocomposite. The processes use silicone surfactants having a molecular weight in the range of 10,000 to 100,000 Dalton to achieve fully exfoliating clay structures. Using these macromolecular silicone surfactants, along with the engineered control of the processing pH and drying stress conditions, this invention provides simple and low-cost methods of making a fully-exfoliated polymer-clay nanocomposite.