High-nickel-content NCA [LiNi0.88C9.Al-09(0.03)] cathode material with non-spherical morphology that consisted of individual primary particles was synthesized at different temperatures. Optimized non-spherical NCA with a mean particle size of 3 pm is compared to conventional spherical NCA [LiNi0.88Co0.09Al0.03] in terms of structural, electrochemical, and thermal stabilities. Non-spherical NCA demonstrates superior cycle performance at both 25 and 45 degrees C. Non-spherical NCA demonstrates superior structural stability with suppressed phase transition from H2 to H3 and anisotropic lattice distortion upon cycling. Electrochemical impedance of non-spherical NCA remained at the same level after 50 cycles, which indicates better structural and electrochemical stabilities. Non-spherical NCA exhibits a higher onset temperature of the exothermic reaction and lower total reaction heat, indicating better thermal stability. Capacity retention of pouch-type cells with non-spherical NCA as the cathode is greater than 91% after 1000 cycles, which shows great potential in the application for a high-energy-density lithium-ion battery for electric vehicles.