In order to improve cyclic capability of Li-ion batteries with NMC cathodes, the core/shell structured powders have been synthesized via a facile and process-controlled oxalate-assisted co-precipitation method. The core and shell morphology is achieved by producing a Ni-rich NMC core in different compositions covered with a Mn-rich NMC-layer. A two-staged synthesis approach has been employed and the process parameters are optimized by means of systematic synthesis protocols. Li-ion batteries having core/shell NMC cathodes yield good electrochemical performance under steady performance tests.