This technique is based on a experimental registration of manifestations of quantum size effects in thin layers on the surface of metal monocrystals continuously for increasing the thickness of the deposited film, starting from submonolayer thicknesses, with using the method of photoelectron spectroscopy with angular resolution (ARPES). The film thickness can be measured with an accuracy of a few tenths of a monolayer and controlled based on the observed spectrum of the quantum electronic states by analysing their energy and quantity. This technique can be used in the manufacture of precision quantum nanoelectronic devices and new nanostructured materials.