Spatially Regulated Silicon Clusters in Trimodal Composite Anodes for High‐Energy Lithium‐Ion Batteries

ABSTRACT Fast‐charging, high‐energy lithium‐ion batteries are central to electrified transportation and grid‐scale energy storage, but their advancement is limited by the instability of high‐capacity anode materials such as silicon (Si). Although graphite (G)‐Si composites offer a practical pathway, their performance remains constrained by uncontrolled Si aggregation and heterogeneous stress evolution. In this study, we introduce a spatial regulation strategy for Si clusters, wherein the electrode architecture creates confined interstitial environments that control Si size and distribution. By integrating G with a dual‐functional organic matrix (cHBC), the system enables continuous ion transport while accommodating mechanical deformation, thereby decoupling electrochemical kinetics from structural degradation. This study demonstrates that electrode performance is governed by spatial architecture rather than compositional optimization alone, providing a generalizable framework for stabilizing high‐capacity materials in next‐generation energy storage systems.