Layered LiNi0.8Co0.15Al0.05O2 (NCA) is a potential cathode material for the next generation of lithium-ion batteries due to its high energy density. However, the rapid attenuation of capacity caused by harmful phase change (H2-H3) and the side reaction between the active material and the electrolyte during the cycle have hindered its further development. In order to solve these problems, the side reaction can be alleviated by fast lithium-ion conductor Li1.5Al0.5Zr1.5(PO4)3 (LAZP) coating on the surface of NCA. At the same time, the doping of Zr4+ also inhibits the generation of harmful phase transition, which improves the cycle life and rate performance of NCA. After 300 cycles at 1C, the capacity loss rate of 1.0 wt% LAZP-NCA is 13.4%, and even at 5C, the capacity loss rate is only 16.3% after 200 cycles. In addition, the full cell composed of 1.0 wt% LAZP-NCA and graphite still has 72.1% capacity retention after 300 cycles at 1C. Therefore, this work provides a new idea for turning NCA into a commercial cathode material for lithium-ion batteries.