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This study investigates the effects of aluminum and nitrogen content on the microstructure, mechanical properties, and tribological performance of high-entropy coatings based on (TiCrAlxNbY)Ny systems. Using a hybrid magnetron sputtering technique, both metallic and nitride coatings were synthesized and evaluated. Increasing the aluminum concentration led to a transition from a crystalline to a nanocrystalline and nearly amorphous (NC/A) structure, with the TiAl0.5CrNbY sample (11.8% Al) exhibiting the best balance of hardness (6.8 GPa), elastic modulus (87.1 GPa), and coefficient of friction (0.64). The addition of nitrogen further enhanced these properties, transitioning the coatings to a denser fine-grained FCC structure. The HN2 sample (45.8% nitrogen) displayed the highest hardness (21.8 GPa) but increased brittleness, while the HN1 sample (32.9% nitrogen) provided an optimal balance of hardness (14.3 GPa), elastic modulus (127.5 GPa), coefficient of friction (0.60), and wear resistance (21.2 × 10−6 mm3/Nm). Electrochemical impedance spectroscopy revealed improved corrosion resistance for the HN1 sample due to its dense microstructure. Overall, the (TiAl0.5CrNbY)N0.5 coating achieved the best performance for friction applications, such as break and clutch systems, requiring high coefficients of friction, high wear resistance, and durability.

Multi-component high-entropy (TiCrAl0.5NbCu)CxNy coatings targeting applications requiring medium-to-high friction and wear-resistant surfaces were fabricated through the co-sputtering of elemental targets in an Ar + CH4 + N2 reactive atmosphere using a hybrid HiPIMS/DCMS technique. Two sets of samples were fabricated: (a) (TiCrAl0.5NbCu)Cx high-entropy carbides (HEC) and (b) (TiCrAl0.5NbCu)CxN0.13 high-entropy carbonitrides (HECN), 0 ≤ x ≤ 0.48. The structural, mechanical, tribological, and corrosion resistance properties were thoroughly investigated. The metallic sample exhibits a single BCC structure that changes to FCC via an intermediary amorphous phase through the addition of C or N to the content of the films. The crystallinity of the FCC phases is enhanced and the density of the films decreases down to 5.5 g/cm3 through increasing the carbon fraction up to 48%. The highest hardness of about 16.9 GPa and the lowest wear rate of about 5.5 × 10−6 mm3/Nm are presented by the samples with the largest carbon content, x = 0.48. We found a very good agreement between the evolution of H/E and H3/E2 parameters with carbon content and the tribological behavior of the coatings. The best corrosion resistance was presented by the low-carbon carbonitride samples, showing a charge transfer resistivity of about 3 × 108 Ω∙cm, which is more than three times larger than that of the metallic HEA. The best tribological characteristics for envisioned application were presented by (TiCrAl0.5NbCu)C0.3N0.13, showing a coefficient of friction of 0.43 and a wear rate of about 7.7 × 10−6 mm3/Nm.