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Fe-doped SiO2/TiO2 composite nanoparticles were directly prepared by sol-gel-hydrothermal process, and characterized by X-ray diffraction (XRD), transmission electron microscope (TEM), thermal gravimetry (TG), X-Ray photoelectron spectroscopy (XPS), and UV-Vis diffuse reflectance spectra (DRS). It was found that the Fe3 + was well dispersed in solid solution of SiO2/TiO2 composite nanoparticles that was about 10 nm with spherical morphology and rich silica layer external surface. It could effectively offer broadband shield for both UVB (290–320 nm) and UVA (320–400 nm). The results of Photodecomposition of methylene blue showed that the photoactivity of Fe-doped SiO2/TiO2 composite was minimized due to the addition of iron ion.