The aim of the work is to obtain and study polymer composite materials based on mixtures of secondary polyolefins and modified polydisperse bentonite clay. The formation features of the structure of mixtures of waste polyolefins in the presence of this-type filler are studied. The data on the changes in the mechanical strength of mixed composites, as well as the results of physico-chemical studies are presented. Mixtures based on waste polymers in the presence of highly dispersed particles of modified polydisperse bentonite are characterized by the improvement of the strength of composites due to increased interfacial interaction in them and by the formation of structure uniformity of the material. This to some extent compensates for the loss of cohesive strength of secondary polymers due to thermal degradation processes. The following conclusions are made: at the phase boundaries, the molecular mobility of polymer chains decreases, which leads to changing the crystallization conditions and to appearing a nonequilibrium stress state; introducing bentonite increases crystalline due to the initiation of physico-chemical interaction; the strength grows due to increased interfacial interaction and structure uniformity; the formation mechanism of a complex of properties of composites consists of two-level adsorption – a modifier on filler particles and active polymer groups on the modified filler surface.