Artificially modulated CrAlN/AlON nanomultilayers were synthesized by direct current reactive magnetron sputtering. The microstructure and mechanical properties were evaluated by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM) and nano-indentation techniques. The crystallization of AlON layer and its influence on the mechanical property of the nanomultilayers were studied. The results revealed that, under the template effect of NaCl structural CrAlN layer, amorphous AlON was forced to crystallize and grew epitaxially with CrAlN layer when AlON layer thickness was below 0.9 nm, leading to an increase of hardness up to 32.8 GPa. With the further increase of the AlON layer thickness, AlON layer gradually transformed into amorphous structure and blocked epitaxial growth of the multilayers, resulting in the decrease of hardness. The effect of CrAlN layer thickness on hardness of CrAlN/AlON nanomultilayers was also investigated. With the decrease of CrAlN layer thickness, the hardness increased gradually. The maximum hardness was 34.7 GPa when CrAlN layer thickness of was 3.0 nm. The strengthen mechanism of CrAlN/AlON nanomultilayers was finally discussed. (C) 2011 Elsevier B.V. All rights reserved.