AbstractAccurately capturing the architecture of single lithium-ion electrode particles is necessary for understanding their performance limitations and degradation mechanisms through multi-physics modeling. Information is drawn from multimodal microscopy techniques to artificially generate LiNi_0.5Mn_0.3Co_0.2O₂ particles with full sub-particle grain detail. Statistical representations of particle architectures are derived from X-ray nano-computed tomography data supporting an ‘outer shell’ model, and sub-particle grain representations are derived from focused-ion beam electron backscatter diffraction data supporting a ‘grain’ model. A random field model used to characterize and generate the outer shells, and a random tessellation model used to characterize and generate grain architectures, are combined to form a multi-scale model for the generation of virtual electrode particles with full-grain detail. This work demonstrates the possibility of generating representative single electrode particle architectures for modeling and characterization that can guide synthesis approaches of particle architectures with enhanced performance.