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This study investigates single and multilayer TiAlN/CrN nanocomposite thin films developed using an RF magnetron sputtering system. The TiAlN and CrN layers showed a high degree of orientation, with the (200) peak being the strongest peak in both layers, and a multilayer structure was clearly observed. The surface roughness analysis using atomic force microscopy (AFM) and cross-sectional transmission electron microscopy (TEM) revealed that the TiAlN/CrN coatings had a smoother surface than the single-layer coatings and minimal intermixing between the two layers. Depth-sensing indentation measurements were used to measure the hardness and Young’s modulus of the coatings, demonstrating that TiAlN/CrN coating had the highest hardness (~16.38 GPa) and elastic modulus (~3.82 GPa) among all the coatings studied. This indicates that the TiAlN/CrN multilayer coating possesses superior mechanical properties due to its interface strength. Our findings suggest that these multilayer coatings have potential applications in tribological and decorative coatings.