CrAlN coatings were deposited on silicon and AISI H13 steel substrates using a modified ion beam enhanced magnetron sputtering system. At the modified ion beam bombardment, the effects of bias voltage and Al/(Cr + Al) ratio on microstructure and mechanical properties of the coatings were studied. The X-ray diffraction data showed that all CrAlN coatings were crystallized in the cubic NaCl B1 structure, showing the (111), (200), and (220) preferential orientation. It is noted that the (111) diffraction peak intensity decreased and the peaks broadened as the bias voltage increased at the same ratio of Al/Cr targets power, which is attributed to the variation in the grain size and microstrain. The microstructure observation of the coatings by field emission scanning electron microscopy cross-section morphology shows that the columnar grain became more compact and dense with increasing substrate bias voltage and Al concentration. At a substrate bias voltage of -120 V and a Al/(Cr + Al) ratio of 40%, the coating had the highest hardness (33.8 GPa) and excellent adhesion to the substrate.