The design of high-performance nanocomposites with improved mechanical, thermal or optical properties compared to starting polymers has generated special interest due to their use in a wide range of targeted applications. In the present work, polymer nanocomposites composed of polyurethane elastomers based on polycaprolactone or polycaprolactone/poly(ethylene glycol) soft segments and titanium dioxide (TiO) nanoparticles as an inorganic filler were prepared and characterized. Initially, the surface of TiO nanoparticles was modified with (3-iodopropyl) trimethoxysilane as a coupling agent, and thereafter, the tertiary amine groups from polyurethane hard segments were quaternized with the silane-modified TiO nanoparticles in order to ensure covalent binding of the nanoparticles on the polymeric chains. In the preparation of polymer nanocomposites, two quaternization degrees were taken into account (1/1 and 1/0.5 molar ratios), and the resulting nanocomposite coatings were characterized by various methods (Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, contact angle, thermogravimetric analysis, dynamic mechanical thermal analysis). The mechanical parameters of the samples evaluated by tensile testing confirm the elastomeric character of the polyurethanes and of the corresponding composites, indicating the obtaining of highly flexible materials. The absorbance/transmittance measurements of PU/TiO thin films in the wavelength range of 200-700 nm show that these partially block UV-A radiation and all UV-B radiation from sunlight and could possibly be used as UV-protective elastomeric coatings.