Water electrolysis plays a vital role in green energy systems and there is an absolute need for abundant, affordable, and effective catalysts for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER). Despite existing challenges, the exploration of transition metal‐based electrocatalysts with superior performance in alkaline water splitting is critical for advancing the hydrogen economy. This study focuses on the electrocatalytic potentials of FeS2, CoSe2, and FeS2@CoSe2 hybrid nanocomposites in response to the increasing demand for sustainable energy production. The prepared materials were synthesized hydrothermally and characterized using X‐ray diffraction (XRD), X‐ray photoelectron spectroscopy (XPS), energy‐dispersive X‐ray spectroscopy (EDX), field emission scanning electron microscopy (FESEM), and transmission electron microscopy (TEM) to examine their structural properties, elemental composition, and morphological features. Notably, the F@C−B nanocomposite exhibited outstanding HER performance, requiring only 97 mV of overpotential to achieve a current density of 10 mA cm−2. Similarly, the F@C−C nanocomposite demonstrated impressive OER efficiency with an overpotential of merely 302 mV at the same current density. The involvement of the Volmer–Heyrovsky mechanism was confirmed through Tafel slope analysis, revealing the improved surface‐active sites and reduced charge transfer resistance of the nanocomposite. The FeS2@CoSe2 nanocomposite with synergistic effects, displayed exceptional electrocatalytic properties, positioning it as a promising candidate for overall water splitting. This work introduces a novel approach to developing highly efficient and cost‐effective electrocatalysts, offering a viable alternative to precious metal‐based counterparts.