A high-nickel layered cathode, LiNi₀.₉₄Co₀.₀₅Te₀.₀₁O₂ (NC95T), was developed to enhance the cycling stability of lithium-ion batteries. This material addresses issues associated with high-nickel content, such as volume changes and oxygen instability, by introducing high-valent tellurium (Te⁶⁺) cations. NC95T exhibits an initial capacity of 239 mAh g⁻¹ and retains 94.5% of its capacity after 200 cycles. When combined with a silicon-carbon anode, it achieves an energy density of 404 Wh kg⁻¹ after 300 cycles. Advanced characterization and theoretical calculations show that Te introduces an ordered microstructure, which accommodates lattice strain and suppresses oxygen loss. This structure enhances oxygen stability and prevents irreversible phase transitions. The material demonstrates excellent structural stability, with minimal lattice strain and no oxygen release during cycling. The ordered Te–Ni–Ni–Te superstructure in the TM layers effectively stabilizes the lattice oxygen, preventing degradation. The study highlights the potential of Te doping in designing high-performance, sustainable cathode materials for lithium-ion batteries.A high-nickel layered cathode, LiNi₀.₉₄Co₀.₀₅Te₀.₀₁O₂ (NC95T), was developed to enhance the cycling stability of lithium-ion batteries. This material addresses issues associated with high-nickel content, such as volume changes and oxygen instability, by introducing high-valent tellurium (Te⁶⁺) cations. NC95T exhibits an initial capacity of 239 mAh g⁻¹ and retains 94.5% of its capacity after 200 cycles. When combined with a silicon-carbon anode, it achieves an energy density of 404 Wh kg⁻¹ after 300 cycles. Advanced characterization and theoretical calculations show that Te introduces an ordered microstructure, which accommodates lattice strain and suppresses oxygen loss. This structure enhances oxygen stability and prevents irreversible phase transitions. The material demonstrates excellent structural stability, with minimal lattice strain and no oxygen release during cycling. The ordered Te–Ni–Ni–Te superstructure in the TM layers effectively stabilizes the lattice oxygen, preventing degradation. The study highlights the potential of Te doping in designing high-performance, sustainable cathode materials for lithium-ion batteries.