Robust π‐Conjugated Hydrogen‐Bonded Organic Framework Nanowires Enable Stable and Fast Potassium Storage

Organic cathodes are considered promising energy storage materials in potassium ion batteries (KIBs) due to their molecular flexibility, cost‐effectiveness, and sustainability. However, challenges such as high solubility and slow reaction kinetics hinder the development of organic molecules for KIBs. Herein, a novel in situ self‐assembly strategy is presented to construct a robust hydrogen‐bonded organic framework cathode (H‐NDA‐G) with extensive π‐conjugated systems and excellent chemical stability. By selecting 2,4‐diaminotriazine as the connecting ligand, which serves both as a hydrogen bond donor and acceptor, the H‐NDA‐G cathode is constructed utilizing its amide reaction with dianhydride and the strong π–π adsorption interactions with graphene oxide (GO). The weak electronic coupling between H‐NDA‐G not only provides charge transfer channels within the framework but also forms an interconnected conductive network through hydrogen bonding and π–π adsorption with the GO, facilitating the redox reactions of K+ within the H‐NDA‐G electrode. Consequently, the H‐NDA‐G cathode exhibits extraordinary performance with a high capacity (120 mAh g−1 at 0.1 A g−1) and cycle life exceeding 1000 cycles at 1 A g−1, demonstrating significant potential for practical applications. This study underscores the potential to enhance the potassium storage capability of organic cathodes by modulating intermolecular forces toward efficient and sustainable KIBs. Through the regulation of intermolecular hydrogen bonding and π–π interactions, a hydrogen‐bonded organic framework composite cathode is constructed, featuring extensive π‐conjugated systems and an ultra‐stable hydrogen bonding network. The weak electronic coupling within this composite cathode not only provides charge transfer pathways but also forms a 3D interconnected conductive network, greatly facilitating the redox reactions of K+ within the electrode.