We demonstrate a selective transition-metal leaching strategy for direct upcycling of Li1-xNi1/3Co1/3Mn1/3O2 (NMC111) into single-crystal Li- and Mn-rich layered oxide (S-LMR). Under optimized processes, ∼80% of Co and Ni are selectively recovered, while residual Mn forms α-MnO2, which serves as a precursor for S-LMR synthesis.