The organophosphorus compound cyclohexylphosphine ((C6H11)PH2, PCH) with trimethylindium (TMI) cleanly forms thin films of crystalline indium phosphide (InP) under pyrolytic CVD conditions. These depositions are shown by Auger electron spectroscopy (AES) and other methods to be polycrystalline InP. Depositions were performed on both silicon (Si) and InP(100) substrates at temperatures and V/III ratios comparable to those employed in literature InP depositions with other phosphorus source compounds. The deposited materials were characterized by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), AES and X-ray thin film diffraction (XRD). The effect of precursor flow rates, V/III ratios, and substrate temperatures on the morphologies and compositions of the deposited InP materials was also investigated for the cyclohexylphosphine-based depositions.