Ni0.8Co0.16Al0.04(CO3)0.19(OH)1.62 was co-precipitated by using a carbonate process. Ni0.8Co0.16Al0.04(OH)2 was also prepared by using a hydroxide process. The carbonate process showed faster particle growth than the hydroxide process. LiNi0.8Co0.16Al0.04O2 (NCA) was obtained from the two precursors and evaluated. NCA from the carbonate process exhibited better electrochemical performances.