© 2022, The Minerals, Metals & Materials Society.The selective leaching of lithium from spent coin-type lithium manganese dioxide CR cells by oxidative leaching and precipitation of Li2CO3 from Li-bearing leach solution has been experimentally and theoretically investigated. The oxidative leaching experiments were carried out using sulfuric acid in the presence of potassium permanganate (KMnO4). The dissolutions of lithium, manganese, nickel, and cobalt were found to be 84.8%, 0.9%, 46.6%, and 9.7%, respectively. The results demonstrated that a considerable amount of manganese and cobalt remained in the leach residue. The Li-bearing leach solution was fed to an impurity removal stage. It was observed that a substantial amount of lithium loss, along with manganese, nickel, and cobalt, was determined at pH 10. At standard temperature and pressure, the species of lithium as a function of pH, lithium concentration, and carbonate concentration was evaluated for the generation of Li2CO3 from the oxidative leach solution. The results revealed that the precipitation of lithium as lithium carbonate is thermodynamically feasible from the solution at high pHs.