The mixed gallium transition-metal complexes [FeCl Ga-2((BU)-B-t)(4)(neol)(2)}] (1) and [M{Ga-2(Bu-t)(4)(neol)(2)}], M = Co (2), Ni (3), Cu (4), have been prepared by the reaction of [Ga-2(Bu-t)(4)(neol-H)(2)] (neol-H-2 = 2,2-dimethyl-propane-1,3-diol) with the appropriate metal halide and Proton Sponge, Compounds 1-4 have been characterized by NMR (3), UV/vis, and IR spectroscopy and magnetic susceptibility (solution and solid state), and their molecular structures have been confirmed by X-ray crystallography. The molecular structure of compounds 1-4 consists of a tetracyclic core formed from two four-membered and two six-membered rings. The central metal atom adopts a square pyramidal (1) or square planar (2-4) geometry. The magnetic susceptibilities for 1, 2, and 4 are as expected for strong ligand field environments, On the basis of spectroscopic and structural data, the [Ga-2(Bu-t)(4)(neol)(2)](2)- ligand appears to be more flexible than other chelating ligands; this is proposed to be due to the flexibility in the O-Ga-O bond angle.