Ni-rich lithium nickel cobalt aluminum oxide (NCA) cathodes, as one of the most promising candidates for the extended electric vehicle applications, have been widely recognized and attracted global interest. However, issues, such as the difficult synthesis of well-regulated morphology particles, poor cognition for electrochemical behavior, and modest electrochemical performance, have put forward a huge challenge for their industrial application. Herein, a hydroxide coprecipitation-calcination two-step continuous synthesis method was employed to prepare NCA cathodes. The key synthesis parameters, including the pH value and ammonia concentration, calcination temperature, and Li/TM ratio were systematically investigated. At the optimal synthesis condition, the obtained precursors displayed good sphericity, narrow size distribution, and desired element composition. After lithiation, the optimized cathode showed a typical layered structure without significant Li/Ni cation mixing. Moreover, the kinetic property and electrochemical behavior of the NCA electrode were analyzed in detail.