Spherical impact indentation tests with different impact angles (90°, 60°, 45°, and 30°) were carried out to understand the impact resistance and interfacial adhesion of zirconia (ZrO2) ceramic coating on steel and aluminum substrates, respectively. A linear rail with an adjustable impact angle was used to guide the slipping impact head to impact the specimen. It is found that the peak impact force for surface damage decreases but the contact indentation becomes longer with decreasing impact angle. Under almost the same peak impact force, the smaller the impact angle, the higher the impulse. The experimental results indicate that the ZrO2 coating on steel substrate has higher impact resistance than that on the aluminum substrate. The cross bonded test results show that ZrO2 coating on both steel and aluminum substrates exhibit excellent interfacial tensile and shear strength.