Developing highly active and robust oxygen evolution reaction electrocatalysts is indispensable to relieve energy crisis. Herein, firstly, the Ni nanocubes precursor as a self-sustaining template is synthesized through a reflow method. Afterward, the nanocubic NiFe bimetallic organic frameworks was formed under the self-assembly approach between the exogenous Fe2+ and released Ni2+ from Ni nanocubes with terephthalic acid organic ligand on the Ni nanocubes precursor, i.e Ni nanocubes@MIL-53(NiFe). The synthesized Ni nanocubes@MIL-53(NiFe) exhibit excellent activity, which only requires the overpotential of 271 and 388 mV to deliver the current density of 20 and 100 mA cm(-2) in alkaline solution (1.0 M KOH). The noticeable catalytic performance can be ascribed to the aspects as following: 1) Ni nanocubes as a template provides a Ni source during the self-assembled process; 2) the metal-metal coupling effect arisen within the Ni and Fe atom is substantially contributed to the oxygen evolution reaction performance; 3) the abundant active sites, enhanced electron transport ability also endow the superior electrocatalytic oxygen evolution reaction activity; 4) rich carboxyl groups in the metal-organic frameworks structure could enhance the hydrophilicity of the catalysts. We anticipate that our study would extend the design and exploration of active metal-organic frameworks on energy conversion field. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.