one important strategy is to prepare micrometer-sized secondary particles composed of agglomerated nanosized primary particles. However, abrupt anisotropic lattice shrinkage occurs along the crystallographic c-axis derived from phases transitions (H2 → H3) at high states of charge, potentially resulting in the generation and buildup of substantial mechanical stress, which is the root cause of microcracks formation, eventual pulverization and electrical isolation of the secondary particles during prolonged cycling. [2] Note that intragranular microcracking has deleterious effects on the performances of nickel-rich cathode, which might provide fast channel for electrolyte infiltration into the particle interior, accelerating parasitic side reactions at the internal electrode/electrolyte interface and associated accumulation of NiO-like detrimental phase and continuous impedance growth. [2b,3] What's worse, a series of other degradation processes could in turn be triggered by this chain-reaction mode. For example, H + species in the electrolyte would severely corrode the surface of reactive particles, giving rise to the dissolution of transition metal (TM) ions, coupled with the release of oxygen, and it further induces profound voltage attenuation and negative safety issues. [3a,4] Therefore, the massive applications of nickel-rich cathodes mainly rely on addressing these bottleneck problems.The discussions above highlight the demand to prevent both physical and chemical degradation of Ni-rich cathodes. Element doping in the bulk phase has been proven to be one of the most effective remedies to inhibit problematic microcracks and stabilize the crystal structure of Ni-enriched layered cathodes. [3b,c,5] In recent years, various ion dopants, such as B, [3b,5a,6] Zr, [5b,c] W, [5d,e] Nb, [5f ] Mg, [5g,h] Ta, [5c] Ce, [5i] Mo, [5j] and Al [5k,7] etc., have been reported to arrest the pernicious effect. For example, Hong and co-workers incorporated element B into the crystal structure of Ni-rich cathode, which remarkably alleviates the inherent microcracking problem. [6] With boron ions introduced into the microstructure, the randomly oriented elongated polygonal primary particles could be transformed into highly textured plate-like microstructures distributed along the radial direction, significantly releasing the interior mechanical strain in the highly delithiated state. Thereby the nucleation and Capacity fading and safety concerns accompanied other deep-rooted challenges have severely hindered commercial development of Ni-rich layered cathodes. Herein, a robust Sr-doped Ni-rich cathode is structurally designed by the reconstruction of the crystal lattice and electronic distribution. Notably, the orbital hybridization between Ni 3d (t 2g ) and O 2p is remarkably reinforced owing to the shortened NiO bond enabled by the electrostatic interaction between Ni and Sr atoms, giving rise to the enhanced crystal structure. Theoretically, the formation energy of oxygen vacancies is greatly increased due to the...