The performance of conventional protective coatings is often constrained by the intrinsic trade-off between hardness and toughness. While high-entropy alloy coatings present a promising alternative, the relationship between their microstructure and properties, along with the underlying strengthening mechanisms, remains insufficiently elucidated. In this study, the high-hardness AlCrNbSiTi coatings were fabricated by arc ion plating under different bias voltages, achieving synergistic optimization of hardness and toughness. The microstructure, phase composition, mechanical properties, and high-temperature oxidation behavior of the AlCrNbSiTi coatings were systematically investigated. The cross-sectional microstructure of the coatings exhibited progressive densification with increasing bias voltages. The coating exhibits the amorphous/nanocrystalline composite structure, which aligns consistently with predictions derived from phase formation parameters. The coatings deposited at −50 V bias exhibited optimal hardness and wear resistance, with values of 26.6 GPa and 1.4 × 10−6 mm3/N·m, respectively. Furthermore, the coatings showed exceptional high-temperature oxidation resistance, maintaining effective substrate protection even after exposure at 1000 °C. The results demonstrate that the AlCrNbSiTi coatings is a promising protective coating with broad industrial application prospects.
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