Oxidation of the nucleophilic nitride, (salen)Mn≡N (1) with stoichiometric Ar3NX initiated a nitride coupling reaction to N2, a major step toward catalytic ammonia oxidation (salen=N,N′‐bis(salicylidene)‐ethylenediamine dianion; Ar=p‐bromophenyl; X=SbCl6− or B(C6F5)4−). N2 production was confirmed by mass spectral analysis of the isotopomer, 1‐15N, and the gas quantified. The metal products of oxidation were the reduced MnIII dimers, (salen)MnCl2 (2) or (salen)Mn(OEt2)2B(C6F5)42 (3) for X=SbCl6− or B(C6F5)4−, respectively. The mechanism of nitride coupling was probed to distinguish a nitridyl from a nucleophilic/electrophilic coupling sequence. During these studies, a rare mixed‐valent MnV/MnIII bridging nitride, (salen)MnV(μ‐N)MnIII(salen)B(C6F5)4 (4), was isolated, and its oxidation‐state assignment was confirmed by X‐ray diffraction (XRD) studies, perpendicular and parallel‐mode EPR and UV/Vis/NIR spectroscopies, as well as superconducting quantum interference device (SQUID) magnetometry. We found that 4 could subsequently be oxidized to 3. Furthermore, in view of generating a catalytic system, 2 can be re‐oxidized to 1 in the presence of NH3 and NaOCl closing a pseudo‐catalytic “synthetic” cycle. Together, the reduction of 1→2 followed by oxidation of 2→1 yield a genuine synthetic cycle for NH3 oxidation, paving the way to the development of a fully catalytic system by using abundant metal catalysis. Store that H2! Oxidation of a simple (salen)Mn≡N resulted in the 6e− nitride coupling reaction, central to NH3 oxidation to N2. A complete synthetic cycle was established with implications for catalytic NH3 oxidation for H2‐storage applications. An unusual mixed‐valent MnV/MnIII species was also isolated and characterized (see scheme).