Hydrogen is considered a very clean and highly available renewable energy resource for the future. Water electrolysis (WE) is a conspicuous promising technology to produce hydrogen on a large scale, without generating carbon dioxide. In this study, we prepared bimetallic NiFe-based metal–organic frameworks (MOFs) integrated with CNTs (NiFe–BTC@CNTs) as highly efficient electrocatalysts for the oxygen evolution reaction (OER) in alkaline water electrolysis. Combining NiFe MOFs and CNTs significantly enhanced the electrochemical performance and structural integrity of the catalyst. The NiFe–BTC@CNT (30 wt.% CNTs) demonstrates a significant low overpotential of 230 mV at 10 mA·cm⁻2, superior catalytic activity with a Tafel slope of 36 mV·dec⁻1, and excellent stability under both constant and dynamic operating conditions. These unique characteristics are attributed to the high surface area and abundant active sites provided by the bimetallic MOF structure, combined with the exceptional electrical conductivity and mechanical strength of CNTs. Furthermore, the integration of CNTs improves the dispersion while preventing the agglomeration of MOF particles, ensuring a more uniform and accessible active surface area. This research highlights the potential of the NiFe–BTC@CNT catalysts as high-performance durable electrocatalysts for sustainable hydrogen production, offering a significant advance in the development of advanced materials for energy conversion and storage applications.