In this study, we propose a new concept for seismic retrofitting using precast modular block walls (PMBWs) to improve and complement the shortcomings of conventional retrofitting methods for reinforced concrete (RC) frames infilled with shear walls, masonry walls, and precast panels. The PMBW retrofitting method maximizes the advantages of factory-produced modular blocks, innovatively enhancing the constructability and integrity of connections between the existing frame and the infilled PMBW. Additionally, the PMBW reinforcement method improves seismic resistance without significantly increasing structural weight, and the required amount of reinforcement can easily be calculated because the strengthening technique involves typical frame infilling. For RC buildings with non-seismic details dominated by shear failure, the application of this seismic reinforcement method readily ensures sufficient strength. A pseudo-dynamic test was conducted on a full-scale two-story frame, based on an existing RC building with non-seismic details, to evaluate the restoring force characteristics, strength enhancement effects, reinforcement strain, and seismic response control capabilities of the PMBW reinforcement system. Based on the pseudo-dynamic test results, the restoring force characteristics for nonlinear dynamic analysis of the PMBW-reinforced specimen were identified. Finally, nonlinear dynamic analysis was conducted using the proposed restoring force characteristics, and the results were compared with the pseudo-dynamic test results. The unreinforced RC frame experienced shear failure at a design basis earthquake magnitude of 200 cm/s2. However, the frame reinforced with the PMBW sustained only minor damage. Even at higher magnitudes under maximum considered earthquake conditions of 300 cm/s2 and large-scale earthquake conditions of 400 cm/s2, only a slight amount of damage was projected from the analysis. Thus, the newly developed PMBW frame infilling system shows great promise for seismic reinforcement.