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Ni-rich cathode materials are a low-cost and high-energy density solution for high-power lithium-ion batteries. However, Li + /Ni 2+ cation mixing and oxygen vacancies are inevitably formed during the high-temperature calcination process, resulting in a poor crystal structure that adversely affects the electrochemical performance. In this work, the LiNi 0.8 Co 0.15 Al 0.05 O 2 cathode material with a regular crystal structure was prepared through oxygen pressurization during lithiation-calcination, which effectively solved the problems caused by the high calcination temperature, such as oxygen loss and a reduction of Ni 3+ . The co-effect of oxygen pressure and calcination temperature on the properties of Ni-rich materials was systematically explored. Oxygen pressurization increased the redox conversion temperature, thus promoting the oxidation of Ni 2+ and reducing Li + /Ni 2+ cation mixing. Moreover, due to the strong oxidizing environment provided by the elevated calcination temperature and oxygen pressurization, the LiNi 0.8 Co 0.15 Al 0.05 O 2 material synthesized under 0.4 MPa oxygen pressure and a calcination temperature of 775 °C exhibited few oxygen vacancies, which in turn suppressed the formation of microcracks during the electrochemical cycling. An additional feature of the LiNi 0.8 Co 0.15 Al 0.05 O 2 material was the small specific surface area of the particles, which reduced both the contact area with the electrolyte and side reactions. As a result, the LiNi 0.8 Co 0.15 Al 0.05 O 2 material exhibited remarkable electrochemical performance, with an initial discharge capacity of 191.6 mA h·g -1 at 0.1 C and a capacity retention of 94.5% at 0.2 C after 100 cycles.