A series of novel alkylxanthato iron(III) precursors [Fe(S2COR)(3)] (R = n-butyl, (1); 2-butyl, (2); 2-methoxyethyl, (3); and 2-ethoxyethyl (4)) have been synthesised and their single crystal X-ray structures have been studied. The complexes were used as single-source precursors for the deposition of iron sulfide thin films as well as nanostructured powders using spin coating technique and solventless thermolysis respectively. Cubic pyrite was obtained using n-butyl xanthato iron(III) and 2-butyl xanthato iron(III) complexes in the temperature range of 200 to 300 degrees C. Structural and morphological investigations using XRD and SEM have been performed to ascertain the crystallinity and morphology of as-prepared thin films and nanostructures. The elemental composition was determined using energy dispersive X-ray (EDX) spectroscopy. The optical band gap energies of pyrite thin films produced by these methods were direct with estimated values in the range 1.6 to 2.3 eV.