Nanolayered multilayer coatings of TiAlN / TiN and TiN / NbN were deposited on Si ͑100͒ substrates at various modulation wavelengths ͑i.e., bilayer thickness, ⌳͒ using a reactive dc magnetron sputtering system. These coatings were characterized using micro-Raman spectroscopy to study the effect of interfaces on the optical-phonon modes. For TiAlN / TiN multilayers, the optical-phonon band shifts to higher frequencies with a decrease in the modulation wavelength. Furthermore, the optical-phonon band shifts to higher frequencies with an increase in the substrate temperature for TiAlN / TiN multilayers deposited at ⌳ = 80 Å. No such shift was observed for single-layer TiN and TiN / NbN multilayer coatings. This observed shift has been attributed to interdiffusion between the layers during deposition, which is more for TiAlN / TiN multilayers as compared to TiN / NbN multilayers. The x-ray-diffraction data showed well-defined satellite reflections for TiN / NbN multilayers at low modulation wavelengths and very weak satellite reflections for TiAlN / TiN multilayers, indicating that interfaces were very broad for TiAlN / TiN multilayers. The nanoindentation data showed no significant improvement in the hardness of TiAlN / TiN multilayers as compared to the rule-of-mixture value, whereas TiN / NbN multilayers showed an improvement in the hardness, which was two times the rule-of-mixture value. The low hardness of TiAlN / TiN multilayers has been attributed to interfacial diffusion.