Lithium-ion batteries are the core components of new energy vehicles. Recycling of spent lithium-ion batteries resources is beneficial for the sustainable development of new energy vehicles. However, the current traditional recycling strategy has the disadvantages of high energy consumption and complex treatment process, which do not meet the requirements of green and energy saving. Here, we report a simpler and greener approach to regenerate spent cathode materials by preoxidation followed by a short annealing approach. The generated cathode material has a good crystal structure and lower Li/Ni mixing. Owing to the stable structure, the generated cathode material exhibits a capacity of 153.82 mA h g–1 at 1C over 2.8–4.3 V with retention reaching 94.74% after 100 cycles. β-NiOOH obtained by preoxidation is beneficial for transformation of the original layered structure in the subsequent short annealing process. The novel approach provides efficient and green ideas for efficient direct regeneration of spent cathode materials.