Iron-based materials have been extensively studied and applied as electrocatalysts. However, the electronic structure of iron itself is not conducive to effectively activating adsorbed intermediates, leading to slower kinetic steps. In this study, a heterogeneous composite catalyst with a nano-sheet array structure consisting of iron boron/sulfide (FeS@Fe2B/IP) was successfully prepared through a two-step process involving boriding and sulfidation of iron plates. The nanosheet array structure provides numerous catalytic active sites, promotes effective contact between electrolytes and catalytic sites, and enhances the apparent reaction rate of the catalyst. Additionally, the heterogeneous interface of FeS/Fe2B plays a crucial role in regulating the electronic structure of the metal Fe site, improving charge transfer rates, and accelerating electrocatalytic reaction kinetics. Ultimately, FeS@Fe2B/IP demonstrates outstanding water splitting performance, with only 177 and 191 mV overpotential providing 10 mA cm−2 toward HER and OER, respectively. Furthermore, it achieves a high current density of 500 mA cm−2 at 473 and 520 mV overpotentials for HER and OER, respectively. In addition to its excellent performance in water splitting applications, a bipolar alkaline cell was constructed using the FeS@Fe2B/IP bifunctional catalyst. This achieved current densities of 10 and 100 mA cm−2 at potentials of 1.63 and 1.75 V. Moreover, the catalytic stability of the FeS@Fe2B/IP system remained consistent for nearly 50 hours at current densities of 10 and 100 mA cm−2. These results confirm that FeS@Fe2B/IP is indeed a high-performance bifunctional electrocatalytic material which can significantly improve energy utilization efficiency in various applications.