The use and scrap of lithium ion batteries, especially power lithium ion batteries in China, are increasing every year. Regeneration of spent battery materials is not only important for environmental protection and resource saving, but also for the production of high value-added materials. In this research, spent power lithium-ion battery cathode material LiNi1-xCoxO2 was acid-leached and a polymetallic leaching solution containing Li, Ni, Co, Al and Cu was obtained. Cu was extracted from the leachate by using CP-150 (2-hydroxy-5-nonyl salicylaldehyde oxime). The optimal conditions were found to be organic: aqueous phase ratio (O/A) = 2:1, extraction agent concentration of 30%, and pH = 3. The precursor was prepared by coprecipitation of the leachate after Cu removal. Then, cathode material of lithium nickel cobalt aluminate LiNi0.8Co0.15Al0.05O2 was synthesized under the optimal conditions of n (precursor): n (lithium carbonate) = 1:1.1, calcination temperature of 800 °C for 15 h. The regenerated LiNi0.8Co0.15Al0.05O2 product prepared under the optimized conditions was in a pure phase with a layered structure and a smooth surface morphology. The first charge specific capacity was 248.7 mAh/g, and the discharge specific capacity was 162 mAh/g. The interfacial impedance was 119 Ω. The 50th-cycle discharge specific capacity was 149.1 mAh/g, and the capacity retention rate was high as 92%. Therefore, the regenerated cathode material exhibited good performance.