The electrochemical removal of abundant and toxic H2S from highly sour reservoirs has emerged as a promising method for hydrogen production and desulfurization. Nevertheless, the ineffectiveness and instability of current electrocatalysts have impeded further utilization of H2S. In this communication, we introduce a robust array of Fe2NiSe4 nanowires synthesized in situ on a FeNi3 foam (Fe2NiSe4/FeNi3) via hydrothermal treatment. This array acts as an active electrocatalyst for ambient H2S splitting. It offers numerous exposed active sites and a rapid electron transport channel, significantly enhancing charge transport rates. As an electrode material, Fe2NiSe4/FeNi3 displays remarkable electrocatalytic efficiency for both sulfide oxidation and hydrogen evolution reactions. This bifunctional electrode achieves efficient electrochemical H2S splitting at a low potential of 440 mV to reach a current density of 100 mA∙cm−2, with a faradaic efficiency for hydrogen production of approximately 98%. These findings highlight its significant potential for desulfurization and energy-efficient hydrogen generation.