Lithium–ion batteries (LIBs) became mainstream power sources for a wide variety of electronic devices and electric vehicle applications. The cost and overall performance of LIBs are primarily dictated by the cathode, which is the heaviest and most expensive component in an LIB. To achieve the recommended threshold for future EVs, Ni-rich, Li[Ni_xCo_y(Mn or Al)_1−x−y]O₂ (NCM or NCA) materials above Ni 90% have become strong cathode candidates because of their high reversible capacities, close to their theoretical values, and relatively low material cost owing to their low Co content. To address the poor durability of Ni-rich NCM cathodes, the introduction of Al into an NCM cathode (NCMA) is a practical strategy to stabilize the host layered structure; consequently, outperforming both NCM and NCA cathodes with the same Ni content. However, the loss of capacity owing to the electrochemical inactivity of Al limits the fraction of the Al dopant that can be introduced. This also limits the usefulness of Al–doping in improving the cycling stability of Ni–rich NCMA cathodes which exhibit rapid capacity fading resulting from the high concentration of unstable Ni⁴⁺ species in the deeply charged state. In this presentation, we report microstructure-tailored NCMA of which the core is encapsulated by a buffer layer. Similar to tempered glass, where a steep thermal gradient during quenching produces different states of stress in the surface and the bulk material, the proposed hybrid cathode structure suppresses the formation of microcracks by creating a non-uniform spatial distribution of the microstrain within the cathode particle, thereby improving its long-term cycling stability.