Masonry was the most used material during the last centuries to build constructions. Most of the existing masonry structures (buildings, bridges, etc.) were built without considering some important structural considerations that are important nowadays. Moreover, due to factors such as the increasing of service loads, materials aging, structural damage, etc., the existing masonry structures require strengthening interventions. The definition of optimal strengthening strategies using traditional and innovative materials is still an important issue of the scientific research. In fact, during the last decade, many researchers focused their attention studying innovative composites materials, such as fiber-reinforced polymers and fiber-reinforced cementitious matrix composites, for the strengthening of existing masonry structures. This research has focused on aspects such as the bond behavior between the substrate and the composite materials, the structural behavior of the strengthened masonry and concrete structures, and the compatibility and reversibility of these materials when bonded to existing substrates. In this study, the bond behavior of a composite material known as steel fiber-reinforced mortar (SFRM), recently used as for the strengthening of existing structures, applied onto masonry structures is analyzed experimentally and numerically. First, the material is characterized experimentally with the aim of getting insight on its behavior and applicability when applied as an innovative technique for the strengthening of masonry and to obtain mechanical parameters required for the numerical models. Mechanical properties of the SFRM studied included flexural and compressive strength, tensile strength, and residual flexural strength. The SFRM bond behavior on masonry substrates was evaluated by means of double shear lap tests. In addition, the experimental tensile and bond behavior of the SFRM is studied numerically through finite-element models validated using the results obtained during the experimental tests. Results show that if an adequate bonded length is provided, the SFRM can fully develop its tensile strength as detachment from the substrate is not observed.