In this work, the NCM523 (LiNi₀.₅Co₀.₂Mn₀.₃O₂) material was regenerated by recovering the precursor materials from spent lithium-ion batteries. The high-purity metal precursors were obtained using a selective oxalate leaching method, which was subsequently processed through ball milling and calcination under various milling and calcination conditions. According to X-ray diffraction, X-ray photoelectron spectroscopy, and electrochemical results, the NCM523 material, characterized by a layered crystal structure, limited cation mixing, and high crystallinity, was obtained by milling Ni0.5Co0.2Mn0.3O and Li2CO3 for 20 hours and subsequently calcining at 750°C. The mechanoregenerated NCM523 exhibited a discharge capacity of ∼155 mAh g⁻¹ at 0.1C, retained 84.6% of its initial capacity after 100 cycles at 0.5C, and demonstrated good rate performance, which was comparable to that of fresh NCM523 material.