Li-rich layered oxides can provide high capacity owing to the simultaneous transition-metal cation and oxygen anion redox. However, irreversible oxygen redox usually occurs during cycling, causing structural collapse, such as the formation of nanovoids, dislocations, and phase transitions. Here, we report the design of an intergrown layered-spinel heterostructure by surface anchoring Al-doped Li₇La₃Zr₂O₁₂ (LLZO) nanodomains to enhance the structural stability. The Al-doped LLZO nanodomains offer a favourable ionic diffusion at the surface and significantly reduce the charge transfer resistance. The abundant local structure suppresses the nanostrain and exhibits minimal cracks in the secondary particles compared to the pristine samples. The target material delivers a discharge capacity of 295.6 mAh·g^–1 with a Coulombic efficiency of 93.5% at 55 °C. After 200 cycles, the structural collapse was significantly reduced. This study provides new insights into the comprehensive design of the electrode/electrolyte interface for transition-metal oxides.