Interface engineering stands to be a successful approach in altering the electronic arrangement and enhancing the inherent activity of heterostructure towards water splitting. Here, we synthesized a two-dimensional copper-ferrous (CF) nanosheets over nickel foam substrate and deposited nickel oxy-hydroxide (NH) nanolayers to form CuFe-LDH/NiOOH (CFN) via a quick and quantifiable chemical approach. The CFN heterostructure enriched with numerous active centers with large surface area, promoted fast faradaic response for water splitting. The CFN electrocatalyst rendered a low overpotential value of 101.2 mV/268.5 mV in 1 M KOH electrolyte to reach 10 mA cm−2 towards hydrogen/oxygen evolution reactions. Additionally, CFN also delivered a mere cell voltage of 1.62 V for achieving a current density of 10 mA cm−2, utilized both anode and cathode in the overall water splitting mechanism. The synergy developed from the seamless interface of CF and NH, enhanced the conductivity, enhanced charge transfer and reaction kinetics at the interface, at a greater extent. Hence, this easy technique of constructing effective electrodes ensures many offerings for energy conversion applications. © 2025 Elsevier B.V., All rights reserved.