A coating process is described that coats a coil-to-coil continuous substrate with a graphene-like coating. The coating process includes cleaning and activating a substrate, applying a graphene oxide dispersion to the substrate, drying the coated sub-strate, and exposing the dried coating to VUV radiation under a dry atmosphere. The atmosphere for the last step includes one or more inert gases and optionally one or more reactive gases to repair defects in the coating and/or to functionalize the coating. This coating process allows for the formation of a polygranular graphene-like coating intimately in contact with the substrate. The graphene-like coating coats the substrate with multiple monolayers of graphene in a continuous manner.