A combined single-source precursor approach has been developed for the deposition of thin films of Cr-doped molybdenum disulfide (MoS₂) by aerosol-assisted chemical vapor deposition (AACVD). Tris(diethyldithiocarbamato)chromium(III) can also be used for the deposition of chromium sulfide (CrS). Films have been analyzed by a range of techniques including scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, Raman spectroscopy, and powder X-ray diffraction (pXRD) to elucidate film morphology, composition, and crystallinity. The presence of Cr in the MoS₂ films produces a number of striking morphological, crystallographic, and nanomechanical changes to the deposited films. The chromium dopant appears to be uniform throughout the MoS₂ from the scanning transmission electron microscopy (STEM) EDX spectrum imaging of nanosheets produced by liquid-phase exfoliation of the thin films in N-methyl-2-pyrollidone.