Using 2-benzylaminopyridine anion as a ligand, we have prepared a family of five- and six-coordinate organometallic complexes of Ga-III and In-III The monomeric nature and unusual distorted square-based pyramidal coordination geometries of the metal centers for M{2-[N(CH2C6H5)]NC5H4}(2)Me (M = Ga, 1; M = In, 2) were confirmed through single-crystal X-ray diffraction analyses. An intermediate in the formation of the gallium complex, Ga{2-[N(CH2C6H5)]NC5H4}Me(2)(OEt(2)), has been characterized spectroscopically. Further reaction of 2 with a third equivalent of amine yields a six-coordinate tris-ligand complex, {2-[N(CH2C6H5)]NC5H4}In-3.