Exploiting highly active, low cost, and stable electrocatalysts for overall water splitting is the central issue for conquering the energy crises and environmental pollution. Herein, an element-incorporation strategy is proposed to synthesize NiFe-based (oxy)hydroxide and selenide nanosheets anchored on a stainless steel mesh (SSM). The (Ni,Fe)OOH/SSM (D-Ni 2 Fe 1 /SSM) obtained via sputtering, alloying, and dealloying strategies and (Ni,Fe)Se 2 (S−Ni 2 Fe 1 /SSM-450) sintering at 450 °C based on the D-Ni 2 Fe 1 /SSM exhibit outstanding hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activities in 1 M KOH, respectively. The preparation of precursor bimetallic hybrid films via sputtering is vital for the subsequent regulation of electronic structures near the active sites between Ni and Fe atoms. D-Ni 2 Fe 1 /SSM requires 176 mV to reach 10 mA cm −2 for the HER, whereas 194 mV is needed for S−Ni 2 Fe 1 /SSM-450 to reach 10 mA cm −2 for the OER. Additionally, these two electrodes are assembled into an alkaline electrolyzer for overall water splitting with a cell voltage of 1.64 V at 10 mA cm −2 and exhibit outstanding stability. The unique roughened nanosheet morphology, large electrochemical surface area, and optimized electronic structures are responsible for the outstanding HER/OER performances.