The new gallium(III) cyclopentadienyl derivatives Ga(C5H4Me)3 and Ga(C5H4SiMe3)3 have been synthesized by metathetical reactions. Subsequent stoichiometric ligand redistribution reactions with GaR3 (R = Me, Et) were used to prepare R2Ga(C5H4Me) as pure single compounds. However, when the syntheses of RGa(C5H4Me)2 (R = Me, Et) and MenGa(C5H4SiMe3)3-n (n =1, 2) by analogous stoichiometric ligand redistribution reactions were investigated, mixtures of compounds were the isolated products. The heteroleptic organogallium compound Me2Ga(C5H4Me) has also been prepared in high yields by using metathetical reactions between Me2GaCl and Li(C5H4Me) in pentane and between Cl2Ga(C5H4Me), formed in-situ from Ga(C5H4Me)3 and GaCl3 in diethyl ether, and LiMe. All pure compounds have been characterized by their physical properties, elemental analyses, NMR spectra, and cryoscopic molecular weight studies.