A 1,4‐Diaza‐3.7‐diphosphacyclo‐otane organometallic bis‐ligand nickel(II) complex [Ni(PPy2Np‐Tol2)2]2+2.[BF4]− on Vulcan XC‐72 (C) functions as both the cathode and anode catalysts in polymer electrolyte membrane fuel cell (PEMFC). In a PEMFC using Ni(Py‐p‐Tol)/C at the anode and Pt/C at the cathode the power density is shown to reach 14.66 mW cm−2, which is the highest power density of the none‐noble organometallic analogs. Based on the data produced using independent physico‐chemical methods, the mechanisms of the hydrogen oxidation and oxygen reduction reactions (HOR and ORR) on the anode and cathode sides of PEMFC, respectively, are reported.