With the rapidly increasing market penetration of electric vehicles, more stringent energy density and cost targets are being required for advanced cathode materials. The current development of Li(Ni_1-x-yMn_xCo_y)O₂ cathodes (NMCs) has focused on increasing Ni content while decreasing expensive Co to maximize the energy density per cathode cost. Now, with the Ni content reaching over 80% in some commercially available NMCs, a fundamental understanding of a true state-of-the-art LiNiO₂ material is essential for the development of next-generation, Ni-based, Co-free cathodes. In a collaborative project supported by the U.S. Department of Energy (DOE), a consortium team of multiple DOE national labs has conducted a deep-dive into the process-structure-electrochemical properties associated with realizing a true LiNiO₂ cathode and its derivatives. In this presentation, high-performance LiNiO₂ cathodes, developed by the consortium team, will be introduced and the critical factors that control their structures and properties will be discussed.