Certain metals and metal alloys can absorb hydrogen through an exothermic chemical reaction, resulting in the formation of metal hydrides. To maintain a rapid charging rate, the produced heat must be extracted as rapidly as it is generated. This study was attempted to evaluate the heat transfer enhancement in a cylindrical hydrogen storage reactor equipped with a central tube for large-scale applications using a 3D transient model. Finite-volume simulations are carried out using the open-source software package OpenFOAM to systematically investigate the impacts of material thermophysical properties, cooling media, and heat exchanger design on the heat transfer behaviors and hydrogen storage rate. The reactor’s performance was evaluated in terms of temperature and total hydrogen mass history profiles, in addition to pressure drop. The findings indicated that the charging time was improved by roughly 86%, compared to the case without thermal enhancement to attain 90% hydrogen storage capacity. A diminished pressure drop was observed between the water-based Al2O3 nanofluid with 5 vol% concentration and pure water at lowered coolant flow velocities, hence enhancing pumping power efficiency. Moreover, the results demonstrated that the storage rate is markedly improved by enhancing the effective thermal conductivity of the hydride bed, increasing the heat exchange area, accelerating the coolant flow rate, and lowering its temperature. The outcomes highlighted the possibility of advancing the current metal hydride reactor for practical application.