The objective of this study is to compare the degradation behaviors of corrosion resistance and mechanical properties of water-based zinc-rich coating/steel substrate system with those of the epoxy zinc-rich coating/steel substrate system with the effects of acid rain over 360 h. The influence of immerse time and pH of electrolyte on degradation of microscopic morphology of two types of coatings was investigated by means of scanning electron microscopy (SEM). Electrochemical test and cross-cut test were conducted to evaluate corrosion resistance and adhesiveness correspondingly. Then three-point bending test and tensile test with digital image correlation (DIC) technology were performed to evaluate the interfacial bonding property of coating/steel substrate systems based on the elastic modulus loss, critical breaking strength and interfacial shear strength. Results show that the corrosion resistance and mechanical properties of epoxy zinc-rich coating corroded at pH 5 and pH 7 are better than those of water-based zinc-rich coating at the same pH. However, the corrosion of water-based zinc-rich coating slowed down at pH 3 electrolyte once the passive film was formed.