This study investigated the flexural strengthening effect of the Thick Hybrid Wall (THW) technique as a seismic retrofit approach for Unreinforced Masonry Wall (URM)-infilled Reinforced Concrete (RC) frames. THW is a strength–ductility-type seismic retrofit technique, which was developed for pilotis-type RC buildings. In this study, the flexural strength and failure mechanisms of URM-infilled RC frames retrofitted using the THW technique were investigated. Consequently, a comprehensive theoretical model was developed to measure the flexural strength, and a previously proposed equation was modified. Additionally, an equation was developed to determine the minimum additional-wall length, and another equation was developed to determine the demand length of the additional wall to obtain the demand flexural strength. These equations enhance the cost-efficiency and reduce the irregularities risks. The interaction between the URM infill and surrounding RC columns was modeled, and a cyclic loading test was performed under the influence of a constant axial force on the four specimens. The results indicate that THW technique changes the failure mechanism of URM-infilled RC frames from shear to flexure and that the retrofitted URM acts as part of the lateral resisting system owing to the active lateral confinement pressure. The accuracy of the analytical models was confirmed via experimental results, and the developed models facilitate the practical implementation of the THW technique on intended frames.