Abstract. Thermoplastic polymer/layered silicate composites were prepared from the same organophilized montmorillonite (OMMT) and four different matrices, polypropylene (PP), the blend of PP and a maleated polymer (MAPP), poly(lactic acid) (PLA) and polyamide (PA) in order to study the effect of their chemical structure and interactions on composite structure and properties. The components were homogenized by extrusion and then specimens were injection molded, which were then characterized by a variety of methods. The results showed that competitive interactions among silicate layers and between the silicate and the polymer determine the extent of exfoliation, and structure. The morphology of the composites is complicated, exfoliation is never complete, besides individual silicate layers, the composite can contain a silicate network, stacks of silicate platelets and larger particles in various amounts. Several local deformation processes can take place around the structural entities as well as in the matrix. Fracture and debonding are the main particle related processes, while cavitation takes place in the polymer, at least in PA and PLA. The macroscopic properties of layered silicate composites are determined by the extent of exfoliation and interfacial adhesion that decreases upon organophilization. Increased reinforcement and improved composite properties can be achieved only by the proper control of all interactions prevailing in the composite.