Layered spheres of NiO/TiO2-SiO2-NiO composition have been synthesized and their physicochemical, optical and structural characteristics have been studied. The obtained material represents particles of spherical shape, containing nickel oxide in the inner layer and having a TiO2-SiO2-NiO outer layer. The application of the production method proposed in this work allows to achieve a uniform distribution of elements and improve the interaction between the inner and outer layers, which increases the stability of the structure to heat treatment at the phase formation stage. According to the results of thermal analysis, the influence of temperatures on the formation of phases of TiO2-SiO2-NiO film was established, the temperature treatment mode was selected, which allows to preserve the spherical shape of the material and to obtain phases of nickel oxide and titanium dioxide with anatase structure under the following conditions: 100 °C - 30 minutes, 200 °C - 30 minutes 300 °C - 30 minutes, 350 °C - 30 minutes, 500 °C - 1 hour. This mode allows to achieve optimal crystallization and adhesion between layers. It was found that the addition of nickel oxide in the composition of the outer layer TiO2-SiO2-NiO influences the optical properties of titanium dioxide and, as a consequence, reduces the energy of the width of the forbidden zone of titanium dioxide to 2.47 eV. This narrowing allows the material to absorb light in the visible range, which significantly expands its potential for photocatalytic processes. The synthesized NiO/TiO2-SiO2-NiO layered structures have a high potential of application in ecology, in such processes as water and air purification, as well as in water treatment processes and destruction of organic pollutants under the influence of electromagnetic radiation in the visible range.