Constructing microstructure from experimental data. Given the anisotropic electrochemical and mechanical properties of NMC cathodes, the present study, along with chemo-mechanical fracture simulations and experimental characterisation studies , demonstrate that regulating the morphology and crystallographic orientation of primary particles can effectively mitigate crystal defect formation, stress concentration, and microcracking in Ni-rich NMC cathodes. Such regulation can significantly improve the rate and cycling performance of composite cathodes. For example, modifying the surface energies through a boron doping strategy can induce the directional growth of primary particles, resulting in NMC secondary particles with radially aligned primary particles . This unique crystallographic texture allows diffusion channels to penetrate directly from the surface to the center, significantly improving the Li-ion diffusion coefficient. Moreover, this radial alignment can effectively alleviate the volume-change-induced stress and intergranular fracture in cathodes . This representative three-dimensional microstructure for chemo-mechanical modeling can be generated based on multimodal microscopy characterisations . Statistical representations of particle microstructures can be derived from X-ray nano-computed tomography data and sub-particle grain representations can be derived from electron backscatter diffraction data .