Metal-halide complexes of a multidentate monoanionic ligand BuN(H)SiMe2N(CH2CH2P'Pr-2)(2), H[N2P2], with Ti, V, Cr, Mn, Fe, Co, and Ni have been isolated and characterized. X-ray crystallographic studies were performed on [N2P2]TiCl2 (3), [N2P2]CrCl2 (5), [N2P2]MnCl (6), [N2P2]FeCl (7), [N2P2]CoCl (8), and [N2P2]NiBr (9), and the results revealed that the [N2P21 ligand exhibits considerable flexibility in the manner in which it binds to first-row metals and that three distinct coordination modes are observed: k(3)-N2P (Ti), k(3) -NP2 (Mn, Fe, Co), and k(4)-N2P2 (Cr, Ni). Electrochemical (CV) data and room-temperature magnetic susceptibilities are also described.