Nanostructured smart coatings (NSC) based on the TiAlSi-CN composite structure elements were deposited using reactive high-power physical vapor deposition (PVD) technique. The advanced modular deposition system included up to 8 high-power magnetron-sputtering-devices (MSD) allowing operate them simultaneously and exceed power density of 120 W/cm2 within each device erosion zone. The novel NSC were deposited on bearing steel 100Cr6 substrates and demonstrated enhanced mechanical and tribological properties compared to the bearing steel commonly used for multifunctional high-tech applications. The deposited NSC containing TiAlSi-CN nanoparticles strengthened by elemental additives Cr and Nb exhibited microhardness as high as 2500 HV values in comparison to 750 HV of 100Cr6 steel substrates. Load-displacement curves follow Meyer’s power-law, with the goodness-of-fit R-squared value of 0.9999 for all samples. Tribological properties were measured under dry friction conditions between the bearing steel ball of Ø 6 mm and the film-samples’ flat surface. Coefficient of friction (CoF) ranged between 0.22-0.56 depending on the sample and load. Tribotracks worn under the friction indenter were too shallow to be evaluated by Mitutoyo profilometer SJ-500. Therefore, the wear rate was estimated as the ball wear of the friction indenter.