It is challenging to design one non-noble material with balanced bifunctional performance for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) for commercial sustainability at a low cost since the different electrocatalytic mechanisms are not easily matchable for each other. Herein, a self-standing hybrid system Ni 18 Fe 12 Al 70 , consisting of Ni 2 Al 3 and Ni 3 Fe phases, was constructed by laser-assisted aluminum (Al) incorporation towards full water splitting. It was found that the incorporation of Al could effectively tune the morphologies, compositions and phases. The results indicate that Ni 18 Fe 12 Al 70 delivers an extremely low overpotential to trigger both HER (η 100 = 188 mV) and OER (η 100 = 345 mV) processes and maintains a stable overpotential for 100 h, comparable to state-of-the-art electrocatalysts. The synergistic effect of Ni 2 Al 3 and Ni 3 Fe alloys on the HER process is confirmed based on theoretical calculation.