This paper reports on the pulsed laser deposition of nanocarbon films on metal and dielectric substrates, using high-purity sacrificial carbon tape as a carbon source on a neutral gas background. The films were characterized by X-ray diffraction (XRD), photoelectron (XPS) and Raman spectroscopy. The XRD and Raman structural analyses revealed that the synthesized films have a graphenic nanocrystalline turbostratic structure, with sp2 clusters about 15–18 nm in size, depending on the laser fluence. A significant decrease in the oxygen and hydrogen contents in the films, in comparison with the target material, was established using XPS, as well as a significant decrease in the sp3 carbon content. The deposited films were found to be similar to reduced graphene oxide (rGO) in composition, with a surprisingly low number of defects in the sp2-matrix. The method proposed in the work may have good prospects of application in the production of energy storage and nonvolatile memory devices.