The aim of this study was to investigate the catalytic activity of hybrid materials of iron supported on hierarchical zeolites in the oxidation reaction of 1-phenylethanol to acetophenone. A greener approach was considered for the preparation of the catalyst and performance of the oxidation reaction. Hierarchical BEA zeolite samples were obtained from an alkaline and a subsequent acid treatment. The materials were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM) and nitrogen adsorption at −196 °C. An iron salt was incorporated onto the hierarchical zeolites by mechanochemical grinding and the catalytic performance of the prepared materials was evaluated towards the microwave assisted oxidation reaction of 1-phenylethanol. The catalyst obtained by Fe immobilization on sample modified by 0.2 M NaOH followed by acid treatment (Fe@BEA0.2AT) is the most promising material with 35% yield and 56% selectivity to acetophenone, allowing five reuse cycles without significant loss of activity and selectivity.