Organo-inorganic nanocomposites with regulated interaction between the components based on sodium silicate, polyisocyanate and promoter of adhesion between organic and inorganic components - gamma-methacryloxypropyl trimethoxysilane have been created. The structure, physical and mechanical properties and chemistry of the formation of organo-inorganic nanocomposites with the help of IR spectroscopy, SEM, and complex of physical-mechanical researches have been investigated. The optimum content of gamma-methacryloxypropyl trimethoxysilane and the ratio of organic and inorganic components in nanocomposites have been determined. The analysis of physical and mechanical properties showed a significant increase in compressive strength (82 MPa) and deformation at compression (31%). Improvement of physical and mechanical parameters of nanocomposites is due to the formation of a more "dense" structure when introducing gamma-methacryloxypropyl trimethoxysilane. The formation of such a structure of nanocomposites in the presence of a promoter of adhesion is confirmed by morphological studies. The obtained results showed the possibility of using gamma-methacryloxypropyltrimethoxysilane as an adhesion promoter in the formation of organo-inorganic nanocomposites with an adjustable interaction between the components.