Zirconium aluminum nitride coatings have been deposited onto Ti-6Al-4V substrates by reactive magnetron sputtering in order to investigate the influence of Al-content on the microstructure and mechanical properties. The morphology and microstructure of the coatings were investigated by field emission scanning electron microscopy (SEM), X-ray diffraction (XRD), and transmission electron microscopy (TEM). Nanoindentation and Vicker’s indentation methods were employed to measure the hardness and toughness of the coatings, respectively. The results show that a structure of single cubic phase with twinning is formed at Al content of x ≤ 0.23, and a two-phase structure of hexagonal and cubic phase is formed at Al content of x ≥ 0.47. Hardness and toughness of the Zr1-xAlxN coatings show similar tendency with the increasing of Al-content. Both of them reach the maximum values at x=0.23 and drop to the minimum values at x=0.47, after that, they slightly increase with the increasing Al-content. The enhanced hardness and toughness achieved at x=0.23 is ascribed not only to single cubic phase structure but also to twinning structure.