This study aimed to develop a highly efficient and stable non-noble metal electrocatalyst to overcome the slow kinetics of the hydrogen evolution reaction (HER) during water splitting. To achieve this, a rapid two-step fabrication strategy was employed: solvothermal deposition of an Fe-based material onto a Ni foam, followed by CO2 laser irradiation. This thermal process drives the in situ growth of a uniform iron carbide phase, creating a hierarchically roughened surface with abundant active sites. Material and electrochemical characterizations revealed that the laser-treated electrode retains the original structure of the substrate, while achieving a threefold increase in the electrochemically active surface area compared to that of a pristine Ni foam. Consequently, the laser-treated Fe3C/Ni electrode demonstrated improved catalytic activity in an alkaline electrolyte, requiring an overpotential of 77 mV to reach a current density of 10 mA/cm−2, whereas the pristine Ni foam requires 215 mV. The electrode also exhibited a low Tafel slope of 108 mV dec−1 and maintained operational stability over 24 h of continuous use. This laser-mediated manufacturing technology offers a scalable, rapid pathway for designing robust, earth-abundant electrocatalysts for large-scale sustainable hydrogen production.