The 17 valence electron (VE) open-shell nickel gallanediyl complex [Cp(Ar)Ni{Ga(nacnac)}] (3, Ar = C5(C6H4-4-Et)5, nacnac = HC[C(Me)N(C6H3-2,6-iPr2)]2), having an unsupported Ni-Ga bond, was synthesized from [Cp(Ar)Ni(μ-Br)]2 (1) by reducing the adduct [Cp(Ar)Ni(μ-Br){Ga(nacnac)}] (2) or, alternatively, trapping the "Cp(Ar)Ni(I)" synthon with Ga(nacnac); spectroscopic and DFT studies showed that the single unpaired electron in 3 resides mainly at the Ni center.