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AbstractWe report a nickel complex for catalytic oxidation of ammonia to dinitrogen under ambient conditions. Using the aryloxyl radical 2,4,6‐tri‐tert‐butylphenoxyl (tBu3ArO⋅) as a H atom acceptor to cleave the N−H bond of a coordinated NH3 ligand up to 56 equiv of N2 per Ni center can be generated. Employing the N‐oxyl radical 2,2,6,6‐(tetramethylpiperidin‐1‐yl)oxyl (TEMPO⋅) as the H‐atom acceptor, up to 15 equiv of N2 per Ni center are formed. A bridging Ni‐hydrazine product identified by isotopic nitrogen (15N) studies and supported by computational models indicates the N−N bond forming step occurs by bimetallic homocoupling of two paramagnetic [Ni]−NH2 fragments. Ni‐mediated hydrazine disproportionation to N2 and NH3 completes the catalytic cycle.