Chemical surface modifications of Al2O3, TiO2, and SiO2 by using diphenylsilane bearing hydrosilyl moieties were investigated by IR spectroscopy and gas chromatography. The hydrosilane was observed to adsorb on the metal oxide surfaces by forming Si-O-metal bonds with generation of hydrogen gas. The results show that hydrosilanes can be used as chemical surface modifiers such as the usual silane coupling agents of silanols, chlorosilanes, and alkoxysilanes.