An Oriented Cu ₃ (HHTP) ₂ @GO Free‐Standing Cathode With Ultrafast Zn ²⁺ Kinetics for High‐Capacity and Durable Flexible Aqueous Zinc‐Ion Batteries

ABSTRACT Flexible aqueous zinc‐ion batteries (AZIBs) offer critical safety and cost advantages for portable/wearable electronics, yet their widespread deployment remains constrained by energy density and cycle stability of cathode materials. Here, we fabricate a flexible free‐standing cathode by integrating 2D conductive metal‐organic framework (2D c‐MOF, Cu 3 (HHTP) 2 ) nanosheets with graphene oxide (GO). Eclipsed stacking in Cu 3 (HHTP) 2 furnishes open 1D pathways for rapid Zn 2+ diffusion, while robust π – π coupling with GO mitigates structural deterioration and volumetric strain during prolonged cycling. The optimized electrode demonstrates outstanding electrochemical performance, delivering a high specific capacity (358.2 mAh·g −1 at 0.2 A·g −1 ), exceptional cycling stability (213.3 mAh·g −1 after 1140 cycles), and ultrafast ion diffusion (10 −10 ‐10 −7 cm 2 ·s −1 ) among the highest reported for MOF‐based cathodes in AZIBs. In situ spectroscopy and theoretical calculations unveil Zn 2+ storage governed by CuO 4 redox centers, while the synergistic Cu 3 (HHTP) 2 @GO heterostructure creates confined microenvironments that boost ion‐insertion kinetics and stabilize the structure. This work establishes a viable pathway for designing durable, high‐capacity flexible electrodes for future energy storage applications.