In this study, we report the synthesis of SiO2@TiO2 core-shell nanocomposite particles by ultrasound irradiation of a mixture of dispersed SiO2 nanoparticles, titanium-tetra-n-butoxide (TBOT), and ammonia in an ethanol-water solution medium. The resulting core-shell nanocomposite particles were characterized by SEM, TEM, FT-IR, XPS, XRF, zeta potential measurements, XRD, and UV-visible spectroscopy. Results showed that TiO2 nanoparticles coated on the surface of SiO2 were 6–10 nm in size and retained an anatase crystalline phase. Zeta potential measurements confirmed that the surface property of the SiO2 changed after TiO2 coating. SiO2@TiO2 core-shell particles demonstrated better decolorization of methylene blue dye compared to commercial TiO2 in aqueous solution under UV light. After treatment, the catalysts were separated with low-speed centrifugation and successfully reused four times without loss of activity. This study may provide some inspiration for the synthesis of other metal oxide-metal oxide core-shell nanocomposite materials through ultrasound irradiation.