Sprayed mortar or shotcrete is a construction technology that could enhance existing masonry buildings' resilience by reinforcing low-safety load-bearing walls. Many factors affect the resistance of shotcrete-reinforced structures. One of the most important is the bond strength at the interface between the shotcrete and the reinforced wall. According to previous technical literature, bond strength usually has two evaluation criteria: shear and tensile strength. The experimental campaign described in this article focused on the bond strength between sprayed mortar and three masonry materials without the influence of normal force or constraint, as well as the roughness of these materials. The analysis of these tests focused on determining the relation between bond strength, roughness, and material strength. The analyses revealed that material strength has a more significant effect on bond strength than roughness, and bond strength is related to shrinkage of the materials. On the basis of previous theories, these researchers found that when there is no obvious influence due to normal force and constraint, the shear strength and tensile strength are different, and the shear strength is likely to be the cohesion force of the two materials. Finally, this article concludes with a novel logarithmic relationship between these strengths.