Catalyst-support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction (OER). Here we modulate the catalyst-support interaction in polyaniline-supported Ni 3 Fe oxide (Ni 3 Fe oxide/PANI) with a robust hetero-interface, which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm -2 and specific activity of 2.08 mA cm ECSA -2 at overpotential of 300 mV, 3.84-fold that of Ni 3 Fe oxide. It is revealed that the catalyst-support interaction between Ni 3 Fe oxide and PANI support enhances the Ni-O covalency via the interfacial Ni-N bond, thus promoting the charge and mass transfer on Ni 3 Fe oxide. Considering the excellent activity and stability, rechargeable Zn-air batteries with optimum Ni 3 Fe oxide/PANI are assembled, delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm -2 . The regulation of the effect of catalyst-support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.