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Three single reinforcement concrete (RC) frames, including 1 reference specimen and 2 specimens strengthened with shear walls, were fabricated and subjected to low cyclic loadings, in order to evaluate seismic performances of strengthened single frame structures with exterior cantilevers. Through comparison and analysis of failure mode, hysteretic behavior, skeleton curve, energy dissipation, strength, and stiffness degradation of the tested frames, the validity of the shear wall-based reinforcement method for single frames was verified. Test results indicate that the stiffness and load-bearing capacities of strengthened frames increased considerably in comparison with the reference frame. A “strong column-weak beam” failure pattern was observed on the cantilever side, and the failure of the shear wall was always prior to the column, which can increase the structural redundancy and improve the failure mechanism and seismic performance of an existing single frame.