The oxidation behaviors of Cr, Cr93.4Al6.6, Cr58.1Al41.9, and Cr34.5Al65.5 coatings, deposited by using multi-arc ion plating technology, at high temperature were studied. The weight gain, oxide thickness, morphology, and phase composition of the coatings before and after oxidation were analyzed in detail. The results show that there is an Al content window available for tuning the oxidation behaviors of the CrAl-based coatings. The Cr93.4Al6.6 coating is considered to be most protective and can effectively improve the high-temperature oxidation resistance of the substrate; whereas, too high an Al content has a harmful effect on the antioxidant properties of the coatings. The oxidation mechanism of Cr and CrAl coatings were also discussed.