In this paper, a potential method for the closed-loop recovery and regeneration of cathode materials from spent lithium-ion batteries (LIBs) is developed to greatly simplify the regeneration process, which successfully removes metal impurities from spent LIBs and synthesis of layered oxide LiNi1/3Co1/3Mn1/3O2 materials. First, the valuable metals (Ni, Co, Mn, and Li) in spent LIB materials are transformed into water-soluble ions based on the synergy between dl-malic acid and glucose. Subsequently, the residual Fe impurities are successfully decreased from the leaching solution by oxidation-precipitation. Prior to the synthesis process, valuable metal ions are immediately precipitated using oxalic acid as a precipitant from the leaching solution into Ni1/3Co1/3Mn1/3C2O4·nH2O with extremely uniform size particles. Furthermore, the LiNi1/3Co1/3Mn1/3O2 materials with an excellent crystal structure are successfully synthesized by adding Li2CO3 as the lithium source after roasting at 500 °C for 4 h and then at 950 °C for 12 h. The regenerated LiNi1/3Co1/3Mn1/3O2 materials demonstrate reliable electrochemical performance. This work clarifies a potential method for the closed-loop recovery resource sustainability of spent LIB materials.