The application and mechanism study of microwave irradiation in traditional industries have attracted considerable attention owing to the unique thermal and athermal effects that could lead to unexpected benefits in high-efficiency and clean production. Herein, we report the investigation of the aluminum tanning under microwave irradiation upon using hide powder and skin pieces, respectively, as simulants of real hide or skin. The aluminum tanning process and the tanned products under microwave heating (MWH) were studied and compared with those of conventional water bath heating (WBH) as the controls. For the tanning system of hide powder, the tanning effluents were analyzed in terms of pH, conductivity, dielectric constant and aluminum content, and the tanned powder was investigated by differential scanning calorimetry (DSC), thermogravimetric (TG) analysis, and FT-IR spectroscopy. For the skin piece system, the pH and aluminum content of tanning effluents were also determined, and at the same time, DSC, TG, SEM, FT-IR and shrinkage temperature were used to illustrate the actions of microwaves on the structure and properties of the tanned pieces. The results show that aluminum reactivity in the penetration and binding process of collagen fibers in hide powder and skin pieces improved using microwave treatment. The residual aluminum content was greatly reduced by microwave heating action, and the increased amount of aluminum with evener distribution was observed in the tanned products. Microwave irradiation also resulted in the tanned products with better thermal stability and thermal decomposition resistance. This work further promotes application of microwave treatments for aluminumbased tanning in leather industry.