Using carbon, nitrogen, and sulfur sourced from thiourea to co-doped TiO2 (C,N,S-TiO2), was prepared via hydrothermal method using precursors of titanyl sulfate TiOSO4, obtained by decomposition of ilmenite ore in Binh Dinh. The material used to make the substrate is glass and distributed onto it is silicone and photocatalytic. The structure and properties of materials system were investigated by modern physicochemical analysis methods including scanning electron microscope (SEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectra, diffuse reflection spectroscopy UV-Vis, transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDX) and nitrogen isothermal adsorption. The photocatalytic ability of materials system after being carried by silicone is demonstrated by decomposing tetracycline (10 mg/L) in aqueous solution with the yield more than 88% efficiency after 6 hours under visible light irradiation. The optimum dose of the photocatalyst was 0.6 g/L under visible light irradiation. The results indicated that C, N, S co-doped TiO2 demonstrated the highest photocatalytic efficiency and a perspective recyclable potential when it is distributed onto silicone.