Thin films of cubic alpha-In2S3 have been deposited on glass, GaAs(100) and InP(111) by low-pressure metal-organic chemical vapour deposition (LP-MOCVD), using novel air-stable precursors of general formulae In(S2CNMeR)(3) [where R = n-Butyl (compound (1)), n-Hexyl (compound (2))]. The predominant phase in all films grown, regardless of substrate or growth temperature, is alpha-In2S3, oriented in the (hhh) direction. The precursor compounds are considerably more volatile than known dialkyldithiocarbamates of indium.