A method of depositing a nanoscale-thin film onto a substrate is disclosed. The method generally comprises depositing a layer of a solid or gaseous state functionalizing molecule onto or adjacent to the first surface of the substrate and exposing the first surface to a source of ionizing radiation, thereby functionalizing the first surface of the substrate. Once the layer of functionalizing molecule is removed, a nanoscale-thin film is then deposited onto the functionalized first surface of the substrate.