We propose radically new periodic structures based on radiation-sensitive and radiation-resistant monocrystals providing, after the action of a given dose of γ-irradiation, purposeful formation of a spatially ordered network of radiation color centers of a given type, an increase in the concentration of centers, and a change in the efficiency of their emission. In order to choose the materials and methods for arranging nanocrystals of a given size on them, we have investigated the specific features of the microstructure and the properties (the absorption, luminescence, and luminescence excitation and polarization spectra) of undoped crystals and films of metal fluorides formed by special methods of thermal vacuum evaporation (TVE) after their γ-irradiation with a given dose. It is shown that nonepitaxial methods of low-temperature TVE-formation of film coatings based on LiF and CaF2 followed by γ-irradiation permit preparing crystalline structures of a given nanosize, a high packing density, and a spatial orientation of irradiated crystals. It has been established that in multilayer LiF TVE-films the specific features of the microstructure provide a high luminescence activity of the radiation F3+ and F2 color centers at 300 K. It is shown that multilayer TVE-films with nanosized radiation-colored LiF crystals are promising for use as integrable sources continuously tunable in the green-red region of the radiation spectrum.