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This article reports on the growth and analysis of CrBN nanocrystalline materials using an ion beam assisted deposition process. In addition, this article addresses the utilization of spectroscopic ellipsometry for in situ analysis of ternary nitrides. Coatings, with a total thickness of 1.5 ±0.2 μm, were deposited at low temperatures (<200 °C) on silicon substrates using ion beam assisted deposition. These coatings were characterized postdeposition using x-ray diffraction (XRD), atomic force microscopy (AFM), x-ray photoelectron spectroscopy (XPS), Auger electron spectroscopy (AES), visible-light spectroscopic ellipsometry (VIS-SE), infrared spectroscopic ellipsometry (IR-SE), and nanoindentation. The primary phases in the films were investigated using XRD. The surface morphology and nanocrystalline nature of the coatings (grain size of 5–7 nm) were deduced using AFM. The elemental composition and phase composition of the samples were determined from XPS and AES measurements and were subsequently deduced from the analysis of the VIS-SE data, and these correlated well. XPS, AES, and IR-SE revealed the crystal structure of the BN phase in the ternary compounds. The correlation of the results from these various techniques indicates that in situ SE may be a potential technique to control the growth of ternary nitride coatings in the future. The mechanical properties of the coatings were evaluated using nanohardness testing. The hardness and elastic modulus were measured to be 19–22 GPa and 250–270 GPa, respectively.