We propose a feasibility of Co-free Ni-rich Li(Ni(1-x)Mn(x))O2 layer compound. Li(Ni(1-x)Mn(x))O2 (0.1 ≤ x ≤ 0.5) have been synthesized by a coprecipitation method. Rietveld refinement of X-ray diffraction and microscopic studies reveal dense and spherical secondary particles of highly crystalline phase with low cation mixing over the whole compositions, implying successful optimization of synthetic conditions. Electrochemical test results indicated that the Co-free materials delivered high capacity with excellent capacity retention and reasonable rate capability. In particular, Li(Ni0.9Mn0.1)O2, which possesses the lowest cation mixing in the Li layers among samples, exhibited exceptionally high rate capacity (approximately 149 mAh g(-1) at 10 C rate) at 25 °C and high discharge capacity upon cycling under a severe condition, in the voltage range of 2.7-4.5 V at 55 °C. The cation mixing in Li(Ni0.9Mn0.1)O2 increased slightly even after the extensive cycling at the elevated temperature, which is ascribed to the structural integrity induced from the optimized synthetic condition using the coprecipitation.