Electrochemical water splitting is a promising method for the generation of "green hydrogen", a renewable and sustainable energy source. However, the complex, multistep synthesis processes, often involving hazardous or expensive chemicals, limit its broader adoption. Herein, a nitrate (NO3-) anion-intercalated nickel-iron-cerium mixed-metal (oxy)hydroxide heterostructure electrocatalyst is fabricated on nickel foam (NiFeCeOxHy@NF) via a simple electrodeposition method followed by cyclic voltammetry activation to enhance its surface properties. The NiFeCeOxHy@NF electrocatalyst exhibited a low overpotential of 72 and 186 mV at 10 mA cm-2 for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively, in 1.0 M KOH. In a two-electrode system, the NiFeCeOxHy@NF obtained a low voltage of 1.47 V at 10 mA cm-2 in 1.0 M KOH with robust stability. Results revealed that the notable activity of the NiFeCeOxHy@NF catalyst is primarily due to (i) hierarchical nanosheet morphology, which provides a large surface area and abundant active sites; (ii) NO3- anion intercalation enhances electrode stability and eliminates the need for binders while simultaneously promoting a strong catalyst-substrate adhesion, resulting in decreased electrode resistance and accelerated reaction kinetics; and (iii) the unique superhydrophilic surface properties facilitate electrolyte penetration through capillary action and minimize gas bubble formation by reducing interfacial tension.