Spherical Li[Ni1/3Co1/3Mn1/3]O2 powders were synthesized from LiOH·H2O and coprecipitated spherical metal hydroxide, (Ni1/3Mn1/3Co1/3)(OH)2 and coated with Al(OH)3. The Al(OH)3-coated Li[Ni1/3Co1/3Mn1/3]O2 showed a capacity retention of 80% at 320mAg−1 (2C-rate) based on 20mAg−1 (0.1C-rate), while the pristine Li[Ni1/3Co1/3Mn1/3]O2 delivered only 45% at the same current density. Also, unlike pristine Li[Ni1/3Co1/3Mn1/3]O2, the Al(OH)3-coated Li[Ni1/3Co1/3Mn1/3]O2 cathode exhibits excellent rate capability and good thermal stability.