TiAlN and CrAlN coatings were prepared using a reactive direct current magnetron sputtering system from TiAl and CrAl targets. Structural characterization of the coatings using x-ray diffraction (XRD) revealed the B1 NaCl structure of TiAlN and CrAlN coatings with a prominent reflection along the (111) plane. The XPS data confirmed the bonding structures of TiAlN and CrAlN single layer coatings. Subsequently, nanolayered multilayer coatings of TiAlN/CrAlN were deposited on silicon and mild steel (MS) substrates at different modulation wavelengths (Λ) with a total thickness of approximately 1.0 μm. The modulation wavelengths were calculated from the x-ray reflectivity data using modified Bragg’s law. TiAlN/CrAlN multilayer coatings were textured along (111) for Λ≪200 Å and the XRD patterns showed the formation of superlattice structure for coatings deposited at Λ=102 Å. The x-ray reflectivity data showed reflections of fifth and seventh orders for multilayer coatings deposited at Λ=102 and 138 Å, respectively, indicating the formation of sharp interfaces between TiAlN and CrAlN layers. The cross-sectional scanning electron microscopy image of TiAlN/CrAlN multilayer coatings indicated a noncolumnar and dense microstructure. A maximum hardness of 39 GPa was observed for TiAlN/C- rAlN multilayer coatings deposited at Λ=93 Å, which was higher than the rule-of-mixture value (30 GPa) for TiAlN and CrAlN. Study of thermal stability of the coatings in air using micro-Raman spectroscopy indicated that the TiAlN/CrAlN multilayer coatings were stable up to 900 °C in air. TiAlN/CrAlN multilayer coatings also exhibited improved corrosion resistance when compared to the MS substrate.