In this work, hydrometallurgical recycling of metals from high-cobalt-content spent lithium-ion batteries (LIBs) from laptops was studied using precipitation and solvent extraction as alternative purification processes. Large amounts of cobalt (58% by weight), along with nickel (6.2%), manganese (3.06%) and lithium (6.09%) are present in LiCoO₂ and Li₂CoMn₃O₈ as prominent Co-rich phases of the electrode material. The pregnant leach solution (PLS) that was generated by leaching in the presence of 10% H₂O₂ using 50 g/L pulp density at 80 °C for 4 h contained 27.4 g/L Co, 3.21 g/L Ni, 1.59 g/L Mn and 3.60 g/L Li. The PLS was subjected to precipitation at various pH using 2 M NaOH but the purification performance was poor. To improve the separation of Mn and other impurities and in order to avoid the loss of cobalt and nickel, separation studies were carried out using a solvent extraction technique using di-(2-ethylhexyl) phosphoric acid (D2EHPA) and bis-(2,4,4-trimethylpentyl) phosphinic acid (Cyanex 272). Overall, this study examines the fundamentals of separating and synthesizing 99.9% pure Co sulfate from leach liquor of spent laptop LIBs with remarkably high cobalt content.