A new type of high-quality zirconium nitride (ZrN) and hydroxyapatite (HA) bionanocomposite was prepared by radio-frequency (RF) magnetron sputtering for biomedical applications. Detailed analysis of this composite coating revealed that a higher substrate temperature (ST) (>300 °C) increased its crystallinity, uniformity, and functional properties. This nanocomposite showed some encouraging functional properties. Mechanical analyses of the nanocomposite showed improved hardness, modulus, and wear resistance, which were found to be due to the increasing volume fraction of ZrN at higher ST. Biomineralization and in vitro cell analysis revealed increased weight gain and enhanced cell activity with increased substrate temperature. Overall, the results of the present study indicate that this nanocomposite coating could become a promising alternative for biomedical applications. © 2014 American Chemical Society.