The cost of replacing failed selective catalytic reduction (SCR) catalysts and their disposal as hazardous solid waste is high. If failed catalysts are recovered and regenerated into new SCR denitration catalysts, the cost of flue gas denitration can be effectively reduced. However, regenerated SCR catalysts have relatively low structural strength and activity and cannot yet form an effective replacement. In this study, aluminum dihydrogen phosphate, aluminum nitrate, and aluminum sulfate were used as structural strengthening agents in the regeneration of SCR catalysts, and over-impregnation, drumming-assisted impregnation, and ultrasonic-assisted preparation techniques were compared. The corresponding regenerated SCR catalysts were then prepared and analyzed for compressive strength, wear strength, H2-TPR, NH3-TPD, and in situ IR. Factors influencing the structural strength, physical properties, and catalytic activity of the regenerated catalysts were investigated. The best results were obtained as follows: compressive strength of 4.57 MPa, wear rate of 0.088% kg-1, and denitration of 58% after 10 min of drumming-assisted impregnation in an aluminum sulfate solution with a concentration of 16%. Based on this, a synergistic method for catalyst activity and structural strengthening was explored to support the design of better SCR catalysts for regeneration.