Slow ionic transport and high voltage drop (IR drop) of homogeneous porous electrodes are the critical causes of severe performance degradation of lithium‐ion batteries at high charging rates. Herein, it is numerically demonstrated that a bio‐inspired vascularized porous electrode can simultaneously solve these two problems by introducing low tortuous channels and graded porosity, which can be verified by porous electrode theory. To optimize the vasculature structural parameters, artificial neural networks are employed to accelerate the computation of possible structures with high accuracy. Furthermore, an inverse‐design searching library is compiled to find the optimal vascular structures under different industrial fabrication and design criteria. The prototype delivers a customizable package containing optimal geometric parameters and their uncertainty and sensitivity analysis. Finally, the full‐vascularized cell shows a 66% improvement in charging capacity compared to the traditional homogeneous cell under 3.2 C current density in a numerical simulation. This computational research provides an innovative methodology to solve the fast‐charging problem in batteries and broaden the applicability of deep learning algorithms to different scientific or engineering areas.
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