To investigate the interfacial bond behaviors between fiber cement mortar and concrete with core drilling and pull-off tests, medium-sized columnar concrete samples enclosed with different strengths of polyvinyl alcohol fiber cement mortar, polypropylene fiber cement mortar, and steel fiber cement mortar were prepared. Core drilling and pull-off tests were conducted on the samples to obtain the pulling force with failure occurring at the interface, and the results of different kinds of samples from pull-off tests were compared with the axial tensile strength of concrete and compressive strength of fiber cement mortar. The results show that the interfacial bond strength between synthetic fiber cement mortar and concrete is higher than that between steel fiber cement mortar and concrete, and that the interfacial bond strength is positively correlated with the axial tensile strength of concrete and compressive strength of fiber cement mortar. There is also a linear correlation between the interfacial bond strength and compressive strength of fiber cement mortar.