In this study, a new heterobimetallic Mo(VI)-V(V) organosilicon Schiff base complex has been prepared and characterized by different techniques, such as FTIR, Raman, MS, ICP-AES, TGA, and XPS. The bimetallic nanocomplex, revealed by TEM images, showed high oxidation stability and desired activity in the aerobic oxidation of a structurally diverse set of benzylic alcohols in ethanol as a safe solvent. Further, oxidation of benzylic hydrocarbons successfully occurred, producing the target compounds in high yields and excellent selectivities. Our results demonstrated a cooperative effect between Mo(VI) and V(V) as redox active sites in an organosilicon Schiff base framework. A facile and practical reusability of the solid catalyst at the end of the reaction was observed.