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Abstract Increasing the thickness of the electrodes is considered the primary strategy to elevate battery energy density. However, as the thickness increases, rate performance, cycling performance, and mechanical stability are affected due to the sluggish ion transfer kinetics and compromised structural integrity. Inspired by the natural hierarchical porous structure of trees, electrodes with bioinspired architecture are fabricated to address these challenges. Specifically, electrodes with aligned columns consist of tree‐inspired vertical channels, and hierarchical pores are constructed by screen printing and ice‐templating, imparting enhanced electrochemical and mechanical performance. Employing an aqueous‐based binder, the LiNi_0.8Mn_0.1Co_0.1O₂cathode achieves a high areal energy density of 15.1 mWh cm⁻²at a rate of 1C at mass loading of 26.0 mg cm⁻², benefitting from the multiscale pores that elevated charge transfer kinetics in the thick electrode. The electrodes demonstrate capacity retention of 90% at the 100th cycle at a high current density of 5.2 mA cm⁻². To understand the mechanisms that promote electrode performance, simplified electro‐chemo‐mechanical models are developed, the drying process and the charge‐discharge process are simulated. The simulation results suggested that the improved performance of the designed electrode benefits from the lower ohmic overpotential and less strain gradient and stress concentration due to the hierarchical porous architecture. 

We developed a model that considers all components of a composite electrode. It integrates particle- and electrode-level behavior and enables simulation of the mechanical behavior of polymeric binders, which is critical for battery degradation.