LiNi 1-x-y Co x Mn y O 2 lithium-ion battery, as the most installed battery of new energy vehicles, is facing the problem of large-scale scrap. In this paper, (Ni 0.1 Co 0.3 Mn 0.6 ) 3 O 4 anode material with a microsphere structure was successfully synthesized by carbonate coprecipitation method, which was obtained by recycling spent LiNi 0.6 Co 0.2 Mn 0.2 O 2 lithium-ion batteries through hydrometallurgy technology. This method eliminates the cumbersome separation steps, reduces the process cost, and realizes efficient recovery of valuable metals. The (Ni 0.1 Co 0.3 Mn 0.6 ) 3 O 4 anode material was characterized by inductively coupled plasma, X-ray photoelectron spectroscopy, X-ray diffraction analysis, scanning electron microscopy, and electrochemical measurements. The results show that (Ni 0.1 Co 0.3 Mn 0.6 ) 3 O 4 anode material has a microsphere structure with high crystallinity and exhibits a high discharge capacity (1575 mAhÁg −1 at 100 mAÁg −1 ) and a good cycling performance (659 mAhÁg −1 at 100 mAÁg −1 after 50 cycles). This work provides a new idea for the recycling of spent LiNi 1-x-y Co x Mn y O 2 batteries.