Metal-organic framework (MOF)-based materials with abundant pore structure, large specific surface area, and atomically dispersed metal centers are considered as potential electrocatalysts for oxygen-evolution reaction (OER), while their ligand-saturated metal nodes are inert to electrocatalysis. In this work, heteroatom doping and interface engineering are proposed to improve the OER performance of Co-MOF-74. Using two-dimensional Ti3C2Tx MXene as a conductive support, Ni-doped Co-MOF-74 (CoNi-MOF-74/MXene/NF) was in situ synthesized through a hydrothermal process, which exhibits excellent OER and hydrogen evolution reaction (HER) properties. For OER, the CoNi-MOF-74/MXene/NF achieves a current density of 100 mA/cm2 at an overpotential of only 256 mV, and a Tafel slope of 40.21 mV/dec. When used for HER catalysis, the current density of 10 mA/cm2 is reached at only 102 mV for the CoNi-MOF-74/MXene/NF. In addition, the two-electrode electrolyzer with CoNi-MOF-74/MXene/NF as both the cathode and anode only requires 1.49 V to reach the current density of 10 mA/cm2. This work provides a new approach for the development of bimetallic MOF-based electrocatalysts.