Peeling failure at the interface is one of the main failure modes for CFRP (Carbon Fiber-Reinforced Polymer)-reinforced steel structures. However, there are very few reported studies on the bond-slip relationship at the CFRP-steel interface. A series of simple shear tests were carried out in the present paper. The influence of the fiber fabric’s width and thickness, the surface roughness of the steel sheet, and the thickness of the adhesive layer on the bonding performance of the CFRP fabric to steel interface was considered. The interface constitutive model and bonding strength model were further established under multiple factors. The results show that with the decrease of the surface roughness, the interface’ ultimate peeling load increases gradually, and the failure has a tendency to develop from a glue-steel interface to a glue-CFRP interface. The test pieces that were subjected to sand blasting obtained the peak value of the ultimate peeling load. This indicates that sand blasting can effectively enhance the interface bonding strength. The theoretical values obtained via the interface prediction model are consistent with the experimental values. This proves that the newly developed interface prediction model can effectively predict the local bonding slip and bonding strength of the interface.