Display omitted •LiNi0.92Co0.04Mn0.04O2 were synthesized using a novel Taylor–Couette Reactor.•Ta-modified LiNi0.92Co0.04Mn0.04O2 shows a bifunctional effect via a controlling suitable amount of Ta and Li-salt.•Ta allows tailoring the primary particles' microstructure, and morphology and forming a coating layer.•The experimental results and DFT calculations were combined to study its effect on the electrochemical performance.•Ta-modified LiNi0.92Co0.04Mn0.04O2 shows excellent electrochemical performance, allowing its EV applications. A novel scalable Taylor–Couette reactor (TCR) synthesis method was employed to prepare Ta-modified LiNi0.92Co0.04Mn0.04O2 (T-NCM92) with different Ta contents. Through experiments and density functional theory (DFT) calculations, the phase and microstructure of Ta-modified NCM92 were analyzed, showing that Ta provides a bifunctional (doping and coating at one time) effect on LiNi0.92Co0.04Mn0.04O2 cathode material through a one-step synthesis process via a controlling suitable amount of Ta and Li-salt. Ta doping allows the tailoring of the microstructure, orientation, and morphology of the primary NCM92 particles, resulting in a needle-like shape with fine structures that considerably enhance Li+ ion diffusion and electrochemical charge/discharge stability. The Ta-based surface-coating layer effectively prevented microcrack formation and inhibited electrolyte decomposition and surface-side reactions during cycling, thereby significantly improving the electrochemical performance and long-term cycling stability of NCM92 cathodes. Our as-prepared NCM92 modified with 0.2 mol% Ta (i.e., T2-NCM92) exhibits outstanding cyclability, retaining 84.5 % capacity at 4.3 V, 78.3 % at 4.5 V, and 67.6 % at 45 ℃ after 200 cycles at 1C. Even under high-rate conditions (10C), T2-NCM92 demonstrated a remarkable capacity retention of 66.9 % after 100 cycles, with an initial discharge capacity of 157.6 mAh g−1. Thus, the Ta modification of Ni-rich NCM92 materials is a promising option for optimizing NCM cathode materials and enabling their use in real-world electric vehicle (EV) applications.