Lead sulfide (PbS) nanoparticles (NPs) of different sizes (2.0 nm - 14.4 nm) have been synthesized in our laboratory. By using those NPs, we formed colloidal films on glass and GaAs substrates employing a specialized supercritical fluid CO2 (sc-CO2) deposition method. The deposited films contain only the PbS NPs and the protecting group of oleic acids and require no polymer matrix. The NP films are solvent free, environmentally stable, and show good adhesion to the substrates. The sc-CO2 deposition process can deposit films ranging in thickness from a few monolayers, in well ordered arrays, up to 0.5 μm or greater. The photoluminescence (PL) properties of these nano-structured films were studied with Fourier transformation infrared spectroscopy from 5 K up to 300 K.