Fast‐Charging and Durable Organic Cathodes Enabled by Two‐Dimensional Supramolecular Polymerization

ABSTRACT Strong demand for fast‐charging and durable batteries drives research into high‐performance organic electrodes beyond conventional layered metal oxides. However, small‐molecule organic electrode materials suffer from sluggish ion diffusion and high dissolution in electrolytes, limiting their practical applications. Here we present sulfur‐heterocyclic extension of redox‐active triptycene tribenzoquinone monomers, enabling two‐dimensional supramolecular polymerization to yield porous multilayer nanosheets with architectural robustness. This supramolecular engineering achieves rapid and stable lithium (Li) storage through cross‐flow ion transport dominated by pseudocapacitance. At a current density of 18 A g −1 , a power‐densed organic cathode (∼42 kW kg −1 ) reaches 76% state‐of‐charge (SoC) only in 44 seconds while retaining 79% of its capacity over 5,000 cycles. Its superior high‐rate performance and cycling stability persist even under cryogenic conditions. We demonstrate its practicability with a Li–organic pouch cell featuring a high areal capacity of 5 mAh cm −2 and 6C‐charging capability to 66% SoC, which fully meets the performance metrics of practical fast‐charging Li‐ion batteries.