Nowadays, carbon enriched nanostructured smart coatings on the carbonitride basis having ultra-low friction and wear, as well as dynamical self-healing properties at high operating loads and temperatures are in the focus of interest, especially for high-tech applications. For instance, one can mention a large variety of machine components operating as friction partners in highly aggressive environment. We propose a novel approach based on modified 3-phase non-stoichiometric carbonitride films to overcome mentioned above limitations. NSC based on carbon nitride constituents (denoted here as CN, C3N4, or CxNy) would theoretically be harder than diamond-type coatings if they could be deposited in the same structure as Si3N4. Producing crystalline carbon nitride coatings is of great interest, though no one has for the time being presented fully crystalline C3N4 coatings. Some specific carbon nitride coatings produced and reported up to now have shown extreme elastic properties combined with relatively high hardness values as (10–50) GPa.