Promising nature-inspired transition metal chalcogenide materials, known for their favorable optical and electrical properties, which are conducive to sustainable solar-based energy and fuels generation, have been identified as an important class of emerging functional materials for future technologies. In this study, thin films of two such ternary sulfides (bornite and chalcopyrite) within the Cu-Fe-S system were successfully synthesized via aerosol-assisted chemical vapor deposition at 450°C for one hour, utilizing iron(III) tris-N,N-diethyldithiocarbamate and copper(II) bis-N,N-diethyldithiocarbamate molecular precursors. The deposited thin films were characterized using powder X-ray diffraction, revealing orthorhombic and tetragonal crystal structures corresponding to bornite (Cu5FeS4) and chalcopyrite (CuFeS2), respectively. Microscale morphology analysis by scanning electron microscopy showcased polycrystalline thin films, with elemental ratios (Cu:Fe:S) consistent with bornite (≈5:1:4) and chalcopyrite (≈1:1:2), as confirmed by X-ray structural characterization. Electrical transport properties were characterized using the four-point probe method, revealing resistivity values of 1.8 × 10-4 Ω-m for bornite and 1.6 × 10-2 Ω-m for chalcopyrite, consistent with bulk material data. Optical energy band gap estimation from Tauc plots of ultraviolet-visible spectroscopy data yielded direct band gap energies of 1.28 eV for bornite and 0.97/1.62 eV for chalcopyrite, indicating their potential as solar-absorbing thin films or photocatalysts for water splitting.