The development of efficient and cost-effective electrocatalysts for the hydrogen evolution reaction (HER) is crucial for renewable energy conversion and storage. Here, we report the synthesis of a mesoporous NiFe2O4/MXene nanocomposite for the alkaline HER. The as-prepared nanocomposite demonstrated a synergistic effect in facilitating the HER, as evidenced by significantly improved electrocatalytic activity compared to individual NiFe2O4 and MXene components. The mesoporous structure of the nanocomposite, derived from the SBA-15 template, provided a large surface area and enhanced mass transport, while the incorporation of MXene as a conductive additive improved the charge transfer kinetics. Based on the results, the NiFe2O4/MXene nanocomposite exhibited a low onset overpotential of −440 mV, a small Tafel slope of 187.5 mV per decade, and long-term stability for the HER in alkaline electrolytes, as opposed to the individual NiFe2O4 or MXene. The enhanced electrocatalytic performance was attributed to the synergistic effect of the unique mesoporous structure, high conductivity, and abundant active sites provided by NiFe2O4 and MXene. However, DFT calculations revealed that more favorable H atom adsorption and activation processes were observed on the surface of the NiFe2O4 (400) plane. Our findings highlight the potential of using templated mesoporous nanocomposites for designing efficient electrocatalysts for the alkaline HER and contribute to the advancement of renewable energy technologies.