The large-scale lithium-ion batteries (LIBs) have begun to retire, and their disposal and reuse is a challenge. Herein, a regenerative and coating synergistic strategy is adopted to achieve the Li3PO4-coated and regeneration of LiNi0.5Co0.2Mn0.3O2 material. The temperature was confirmed great influence to regenerate. The sample of 850 °C has the best cycle performance and rate performance, and the capacity retention rate is more than 80% after 100 cycles at 1 C. The recovery of material properties is due to structural repair and Li3PO4 coating. The coating and regeneration strategy can be applied to the regeneration of other cathode materials and provides guidance for the treatment and reuse of waste LIBs electrolyte.