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Designing a high-performance electrocatalyst that operates with photon-level energy is of the utmost importance in order to address the world's urgent energy concerns. Herein, we report IrNi nanoparticles uniformly distributed on cost-effective activated carbon support with a low mass loading of 3% by weight to drive the overall water splitting reaction under light illumination over a wide pH range. The prepared IrNi nanomaterials were extensively characterized by SEM/EDX, TEM, XRD, Raman, and UV-visible absorption spectroscopy. The experimental results demonstrate that when the Ir:Ni ratio is 4:1, the water splitting rate is high at 32 and 25 mA cm−2 for hydrogen (at −1.16 V) and oxygen evolution reactions (at 1.8 V) in alkaline electrolyte, respectively, upon the light irradiation (100 mW cm−2). The physical and electrochemical characterization of metal and alloy combinations show that the cumulative effect of relatively high crystallinity (among the materials used in this study), reduced charge recombination rate, and improved oxygen vacancies observed with the 4Ir1Ni@AC electrode is the reason for the superior activity obtained. A high level of durability for hydrogen and oxygen evolution under light illumination is seen in the chronoamperometric study over 15 h of operation. Overall water splitting examined in 0.1 M of NaOH medium at a 50 mV s−1 scan rate showed a cell voltage of 1.94 V at a 10 mA cm−2 current density. [ABSTRACT FROM AUTHOR]