Single-crystal NCMs show properties of good cyclability and high safety, and considers as promising cathode materials for next generation lithium batteries. But industrial production of single-crystal NCMs should overcome problems of lengthy production steps, high production costs and poor consistency. In this work, a Ni-Co-Mn ternary MOF has been developed for NCM cathode materials preparation. The MOF derived precursors show high activity and can be used to prepare single-crystal NCM111 (SC-NCM) in a regular sintering process. As-prepared SC-NCM cathode materials show an average particle size of 400 nm, reveal a polyhedral structure with smooth surface, and can be applied as a high-voltage cathode with excellent cyclability and high specific capacities. Specifically, it is delivery a high discharge capacity of 172 mAh g⁻¹ and maintains 156 mAh g⁻¹ after 50 cycles in a large potential range of 2.8–4.6 V at a high current of 1 C; it also reveals a good capacity retention of 88.3 % after 600 cycles. The enhanced electrochemical performance can be attributed to the SC-NCM reveals a good microstructural stability, which prevents the unexpected structural degradation and microcrack generation during battery cycling. This work provides a new method to synthesis the high-quality single-crystal NCM materials with good electrochemical performance.