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Layered LiNixCoyMn1-x-yO2(NCM, or NCMxy(1-x-y)) is a dominant family of cathode materials for lithium-ion batteries (LIBs) due to its high energy density. Among all NCM cathode materials, NCM622 possess the optimal energy density at high potential (≥ 4.6V vs.Li/Li+). However, the practical application of NCM622 at high voltage (≥ 4.6V) is limited by its parasitic reactions and associated safety concerns. Completely physical isolation has been considered as the main approach to mitigate the parasitic reaction. It has also been previously demonstrated that the interface reaction has active site selectivity, and that the reactivity of the active sites can effectively suppressed by blocking the chemically active sites. Herein, a targeted masking by LiFePO4@C nanoplates is reported to unlock the stable performance of NCM622 up to 4.6V vs.Li/Li+. The (targeted masked-NCM622)|graphite pouch cell shows 86.5% capacity retention after 1000 cycles and its maximum temperature during thermal runaway is dramatically reduced from 570 °C to 415 °C. Systematic in/exsitu characterizations, first-principles calculations and half/pouch cell evaluation prove that PO43-is preferentially adsorbed on transition metal sites, stabilizing both the transition metal ions and oxygen ions on the surface against the ethylene carbonate-containing traditional electrolyte even under high voltage (≥ 4.6V vs.Li/Li+). This work opens up new venue for rational design of high-performance cathode materials through a low-cost and scalable decoration process, and reveal a new understanding of interfacial activity of materials.