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[Display omitted] • A rational coating-integrated-into-synthesis design was used to prepare surface Ti-enriched NMC811 material. • The Ti substitute has a unique tri-valence (Ti3+) in a gradient surface distribution. • The surface Ti-enriched NMC811has high cationic ordering both in the bulk and surface. • Theoretical simulations certify enhanced stability of lattice oxygen for the NMC811#Ti material. • The NMC811#Ti cathode shows improved cycling performance and thermal/ storage stabilities. High-Ni cathodes are being intensely pursued worldwide for electric vehicles and other energy-dense applications due to their high capacity and low cost. However, structural instabilities during electrochemical cycling and when subjected to thermal treatment have been the major issues hindering their practical deployment. We here report a rational design of coating-integrated-into-synthesis protocol for fabricating surface Ti-enriched LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811#Ti) material. The coating to intermediates is crucial to obtain high structural ordering, both in the bulk and surface of high-Ni cathodes, and the Ti substitute has a unique tri-valence (Ti3+) in a gradient surface distribution. The simulations of projected density of states in the atomistic understanding further certify significantly enhanced stability of lattice oxygen for the NMC811 through such a Ti3+-based structure reinforcement. Consequently, the NMC811#Ti cathode delivers a high capacity up to 200 mAh g−1 at 0.1 C, along with superior stabilities during air-storage and thermal treatment (up to 297 °C at the fully charged state under differential scanning calorimetric measurements). The corresponding NMC811#Ti||graphite full cell exhibits a desired 83.6 % capacity retention after 1000 cycles at 0.5 C in a voltage range of 2.8–4.3 V. This work demonstrates a delicate surface reinforcement to stabilize high-Ni cathodes for long-life and safe lithium-ion batteries. [ABSTRACT FROM AUTHOR]