Electrode architectures significantly influence the electrochemical performance, flexibility, and applications of lithium‐ion batteries (LiBs). However, the conventional bar coating for fabricating electrodes limits the addition of customized architecture or patterns. In this study, as a novel approach, patterns are integrated into electrodes through large‐scale roll‐to‐roll (R2R) flexographic printing. Additionally, flexible, recyclable, and biodegradable paper are innovatively used as a printing substrate during printing LiBs manufacturing, which exhibited superior printability. Moreover, the paper is modified with a thin‐layer Al2O3 to function as the separator in the printed LiB. The Al2O3‐coated paper enables an admirable wettability for printing, excellent mechanical properties for high‐speed R2R manufacturing, and outstanding thermal stability for the safe and stable operation of LiBs. The assembled paper cells exhibit nearly 100% discharge capacity retention after 1000 cycles at 3 C and outstanding rate performance. This work inspires future large‐scale microbatteries manufacturing integrated with high‐resolution architecture designs.

Achieving high energy density and fast charging of lithium‐ion batteries can accelerate the promotion of electric vehicles. However, the increased mass loading causes poor charge transfer, impedes the electrochemical reaction kinetics, and limits the battery charging rate. Herein, this work demonstrated a novel pattern integrated stamping process for creating channels in the electrode, which benefits ion transport and increases the rate performance of the electrode. Meanwhile, the pressure applied during the stamping process improved the contact between electrode and current collector and also enhanced the mechanical stability of the electrode. Compared to the conventional bar‐coated electrode with the same thickness of 155 μm (delivered a discharge capacity of 16 mAh g−1 at the rate of 3 C), the stamped low‐tortuosity LiFePO4 electrode delivered 101 mAh g−1 capacity. Additionally, water was employed as a solvent in this study. Owing to its eco‐friendliness, high scalability, and minimal waste generation, this novel stamping technique inspire a new method for the industrial‐level efficient roll to roll fabrication of fast‐charge electrodes.

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The development of fast-charging technologies is crucial for expediting the progress and promotion of electric vehicles. In addition to innovative material exploration, reduction in the tortuosity of electrodes is a favored strategy to enhance the fast-charging capability of lithium-ion batteries by optimizing the ion-transfer kinetics. To realize the industrialization of low-tortuosity electrodes, a facile, cost-effective, highly controlled, and high-output continuous additive manufacturing roll-to-roll screen printing technology is proposed to render customized vertical channels within electrodes. Extremely precise vertical channels are fabricated by applying the as-developed inks, using LiNi 0.6 Mn 0.2 Co 0.2 O 2 as the cathode material. Additionally, the relationship between the electrochemical properties and architecture of the channels, including the pattern, channel diameter, and edge distance between channels, is revealed. The optimized screen-printed electrode exhibited a seven-fold higher charge capacity (72 mAh g −1 ) at a current rate of 6 C and superior stability compared with that of the conventional bar-coated electrode (10 mAh g −1 , 6 C) at a mass loading of 10 mg cm −2 . This roll-to-roll additive manufacturing can potentially be applied to various active materials printing to reduce electrode tortuosity and enable fast charging in battery manufacturing.

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