A new redox-active, tris(amido) ligand platform, bis(2-isopropylamino-4-methoxyphenylamine [NNNcat](3-), has been prepared and used in the preparation of tantalum(V) complexes. The ligand was prepared in its protonated form by a three-step procedure from commercially available 4-methoxy-2-nitroaniline and 1-iodo-4-methoxy-2-nitrobenzene. Direct reaction of (NNNcat]H-3 with TaCl2Me3 afforded five-coordinate [NNNcat]TaCl2 (1), which accepted the strong sigma-donor ligand (BuNC)-Bu-t to form the six-coordinate adduct [NNNcat]TaCl2((CNBu)-Bu-t) (2). Complex 1 is formally a d(0), Ta-v complex; however, one- and two-electron reactivity is enabled at the metal center by the redox-activity of the ligand platform. Complex 1 was oxidized by one electron to afford the radical species [NNNsq center dot]TaCl3 (3), which was characterized by solution EPR spectroscopy. Cyclic voltammetry studies of complex 3 showed clean one-electron oxidation and reduction processes at 0.148 and -0.324 V vs [Cp2Fe](+/0), indicating the accessibility of three oxidation states, [NNNcat](3-), [NNNsq center dot](2-), and [NNNq](-), for the metallated ligand. Complex 1 also can undergo two-electron reactions, as evidenced by the reaction with nitrene transfer reagents to form tantalum imido species. Thus 1 reacted with organic azides, RN3 (R = Ph, p-C6H4Me, p-(C6H4Bu)-Bu-t), to form [NNNq]TaCl2(=NR) (4). Similarly, the tantalum diphenylmethylidenehydrazido complex, [NNNq]TaCl2(=NNCPh2) (5), was formed by reaction of 1 with the diazoalkane, N2CPh2.