Unsaturated polyester (UP) systems give rise to numerous possible approaches in synthesizing nanocomposites. A simultaneous mixing method was used to synthesize UP-resin/organo-clay nanocomposites. The effects of various mixing processes, using several organically-modified clay types, were investigated. The incorporation of these organo-clays resulted in an intercalated structure, the extent of which depended mainly on the type of the clay organic treatment. Organo-clays that exhibited the highest intercalation levels were further studied using a sequential mixing method. The UP-alkyd (without styrene) was mixed with different organo-clays. Processing parameters such as mixing modes, applied shearing levels, clay contents, and mixing-temperatures were investigated. Prolonged high shear levels promoted the intercalation and exfoliation of the silicate layers, resulting in a better dispersion of clay particles. The high shear levels effects were achieved by vigorous mechanical mixing and were intensified by using large amounts of clay and optimized matrix viscosity. Rheological studies of the nanocomposites were found complementary and in correlation with morphological and thermal characterization. This methodological approach provides a basis for understanding the structuring processes involving the formation of the UP/clay nanocomposites and establishing materials-processing-structure interrelations. (C) 2005 Society of Plastics Engineers.