As the cathode ternary activated materials with high content of nickel have been widely used in lithium-ion batteries, the recycling of the spent cathode materials has been paid worthy attention. In this work, the sulfate solution with Li, Ni, Co and Mn elements was formed by dissolving the spent LiNi0.5Co0.2Mn0.3O2 cathode materials in 20% sulfuric acid and 30% H2O2, assisted with reflux at 90 °C for 1 h. Based on the above solution, the precursor (Ni0.5Co0.2Mn0.3(OH)2), along with the lithium and sodium sulfates mixture solutions were prepared by co-precipitation at 55 °C. Then Li2CO3 powders and sodium sulfate solution were obtained through evaporating filtered solution separated from the preparation of the precursor and added an amount of Na2CO3, with the removal of 30% water and separation at about 70 °C. The purity of recovered Li2CO3 is about 99.5%. The residual concentrations of Ni, Co and Mn in the filtered solution separated from the preparation of precursor are only 0.041, 0.025, 0.038 ppm left, respectively. The prepared cathode material LiNi0.5Co0.2Mn0.3O2 from the precursor exhibits good cycle performance and shows a stable discharge capacity of 140 mAh g−1 at a current rate of 100 mA g−1 between 2.8 and 4.2 V.