Herein, we reported a facile strategy to prepare bimetal-polyphenol complexes coating on carbon nanotube (CNT) as a highly efficient OER catalyst. Tannic acid was used as an organic ligand to simultaneously coordinate with Ni and Fe ions and at the same time wrapped the surface of CNT. The obtained Ni3Fe/TA@CNT catalyst showed superior catalytic activity with a low overpotential of 287 mV to reach the current density of 10 mA cm(-2) under a small Tafel slope of 70.24 mV dec(-1) and exhibited persistent stability in alkaline environment. Experimental results and density functional theory (DFT) calculations revealed that the electron transfer from CNT to Ni3Fe/TA on the heterointerface modified the local electronic environment of the catalyst at atomic level and decreased the binding energies of adsorbed species, thus greatly accelerating the OER kinetic process and enhancing electrocatalytic activity. (C) 2020 Elsevier Inc. All rights reserved.