Concentration-gradient layered Li[Ni 0.8 Co 0.2 ] 0.7 [Ni 0.2 Mn 0.8 ] 0.3 O 2 oxide with Ni-rich in the core and Mn-rich in the surface region has been synthesized through a condition-controlled tank reactor reaction. While the Ni-rich core facilitates high capacity, the Mn-rich surface enables good cyclability and thermal stability. The concentration-gradient sample exhibits a higher capacity of 204 mA h g-1 at C/5 rate with superior cyclability and thermal stability compared to the constant-concentration LiNi 0.62 Co 0.14 Mn 0.24 O 2 sample, which has the same net Ni, Co, and Mn contents as those present in the concentration-gradient sample. The concentration-gradient sample was also coated with a thin layer of Al 2 O 3 on the surface to stabilize the electrode/electrolyte interface and thereby further improve the electrochemical performance. Both the structural (gradient structure) and surface (Al 2 O 3 coating) modifications help suppress side reactions between electrode and electrolyte and reduce the decline in voltage during cycling. The Al 2 O 3-coated concentration-gradient sample exhibits improved long-term cyclability, rate capability, and thermal stability compared to the pristine uncoated sample.