Ion transport kinetics is identified as the major challenge of thick electrode design for high‐energy‐density lithium‐ion batteries. The introduction of vertically‐oriented structure pores, which provide fast transport pathways for Li+, can maximize the rate‐performance of electrodes while holding a high energy density. To overcome the harsh manufacturing requirements of traditional template‐based methods for the oriented‐pore electrodes, a template‐free strategy is developed to meet the large‐scale fabrication demand, in which controllable oriented microchannels are facilely constructed by vertically aggregated bubbles generated from thermal decomposition. The proposed method is demonstrated to be applicable for different active materials and compatible with industrial roll‐to‐roll manufacturing. The oriented‐pore electrodes exhibit a seven times higher capacity at 5C rate and show double the power density relative to the state of the art while maintaining a high level of energy density. The balance between the ion transport kinetics through the channels and in the matrix manifests an optimal design of the electrode structures, enabling the desired superior performance of the electrodes toward practical applications.

High‐energy density and ultra‐long cycling lifespan are of great significance in pursuit of practical lithium–sulfur (Li‐S) batteries, in which the construction of ultrathick, high‐areal‐capacity, and stable‐cycling sulfur cathodes remains challenging. Here, a unique layered reinforced concrete structure (LRCS) is reported by integrating an ice‐template method with incorporating carbon fibers in the thick electrodes for Li‐S batteries. The LRCS enables aligned through‐channel structure and intertwined conductive network, which lead to both fast kinetics of ions/electrons transport and strengthened electrode integrity to tolerate the volume change during cycling and the dimensional deformation under a high compaction density. Benefiting from the unique structure, the ultra‐thick Se0.05S0.95 @ pPAN cathode (20.2 mg cm−2) delivers a high capacity of 10 mAh cm−2 and excellent capacity retention of 80.8% over 140 cycles at a low electrolyte‐to‐sulfur ratio of 2 and a negative‐to‐positive capacity ratio of 2.7, corresponding to a calculated energy density of 390 Wh kg−1. This investigation not only provides guidance for the design of thick sulfur electrodes but also paves the way for the development of practical Li‐S batteries.

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