This paper describes the redox chemistry of a tetrazene ligand on (beta-diketiminato) iron complexes. Addition of 1-adamantyl azide to an iron(I) source gives the tetrazene complex (LFe)-Fe-Me(AdNNNNAd), most likely through an imidoiron(III) intermediate. Spectroscopic, magnetic, crystallographic, and computational investigations of the tetrazene complex show that one unpaired spin occupies a primarily ligand-based orbital, and is antiferromagnetically coupled to a high-spin iron(II) ion to give an S = 3/2 ground state. Reversible single-electron reduction occurs at the ligand singly occupied molecular orbital (SOMO), affording a dianionic tetrazene ligand while leaving the metal oxidation state and spin state unchanged.