AbstractHerein, we reported the efficient method for synthesis of aldehydes, ketones and carboxylic acids from olefins catalyzed by inorganic‐ligand Fe (III) catalyst, (NH4)3[FeMo6O18(OH)6]. This transformation features sustainable conditions and utilizes commercially available H2O2 as the sole oxidant and CH3CN/ AcOH as the solvent. The simple synthesized catalyst has high efficiency towards the reactions under mild conditions and can be recycled at least six times with keeping stable activity. At the same time, the controllable products in the reaction have the potential for industrial application.