The ternary chalcopyrite semiconductor Cu(In/Ga)(Se/S) 2 is currently used as an absorber layer in high efficiency thin film solar cells. In this study, various types of I-III-VI (I = Cu, III= Ga or In, VI = S or Se) thin films (CuGaS 2 , CuInS 2 and CuInSe 2 ) were prepared from a series of organometallic precursors, M[(S/Se) 2 CNMeR], (M = Cu, In, Ga; R = alkyl) by aerosol-assisted chemical vapour deposition (AACVD). In contrast to the metal alkyl compounds, MR 3 (M = In and Ga; R = alkyl), which are pyrophoric, the precursors are easy to synthesize by one-pot reactions and are air stable. The optimum growth temperature for the preparation of these films on glass substrates using aerosol-assisted chemical vapour deposition (AACVD) was found to be above 400 °C in terms of crystallinity, although deposition does occur at lower temperatures. The films have been characterised using XRPD, SEM and EDS. SEM analyses show all films are microcrystalline. XRPD results show evidence of the crystalline nature of theses films. The results of this comprehensive study are presented and discussed.