LiNi0.8Co0.15Al0.05O2 cathode material for lithium-ion batteries is synthesized by sintering the precursor Ni0.8Co0.15Al0.05OOH, which is prepared from the corresponding metal sulphates solution by a co-oxidation-controlled crystallization method. The effects of calcination temperature and time on the electrochemical performance of the material are investigated on the basis of TG-DSC analysis. XRD analyses show that the powders obtained by calcination at 700°C for 6h have the best-ordered hexagonal layer structure. SEM images show that these powders are spherical particles with diameter in the 5–12μm range. The XPS measurement and the chemical titration display that Ni ions of these powders are in the form of Ni3+. The charge–discharge tests demonstrate that these powders have the best electrochemical properties, with an initial discharge capacity of 196.8mAhg−1 and capacity retention of 96.1% after 50 cycles when cycled at a current density of 0.2C between 2.8 and 4.3V. Besides, these powders have also exhibited excellent rate capability and high-temperature performance.