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Abstract Matching the capacity of the anode and cathode is essential for maximizing electrochemical cell performance. This study presents two strategies to balance the electrode utilization in zinc ion supercapacitors, by decreasing dendritic loss in the zinc anode while increasing the capacity of the activated carbon cathode. The anode current collector was modified with copper nanoparticles to direct zinc plating orientation and minimize dendrite formation, improving the Coulombic efficiency and cycle life. The cathode was activated by an electrolyte reaction to increase its porosity and gravimetric capacity. The full cell delivered a specific energy of 192 ± 0.56 Wh kg⁻¹at a specific power of 1.4 kW kg⁻¹, maintaining 84% capacity after 50,000 full charge-discharge cycles up to 2 V. With a cumulative capacity of 19.8 Ah cm⁻²surpassing zinc ion batteries, this device design is particularly promising for high-endurance applications, including un-interruptible power supplies and energy-harvesting systems that demand frequent cycling. 

Abstract Supercapacitors have emerged as an important energy storage technology offering rapid power delivery, fast charging, and long cycle lifetimes. While extending the operational voltage is improving the overall energy and power densities, progress remains hindered by a lack of stable n‐type redox‐active materials. Here, a new Faradaic electrode material comprised of a narrow bandgap donor−acceptor conjugated polymer is demonstrated, which exhibits an open‐shell ground state, intrinsic electrical conductivity, and enhanced charge delocalization in the reduced state. These attributes afford very stable anodes with a coulombic efficiency of 99.6% and that retain 90% capacitance after 2000 charge–discharge cycles, exceeding other n‐dopable organic materials. Redox cycling processes are monitored in situ by optoelectronic measurements to separate chemical versus physical degradation mechanisms. Asymmetric supercapacitors fabricated using this polymer with p‐type PEDOT:PSS operate within a 3 V potential window, with a best‐in‐class energy density of 30.4 Wh kg⁻¹at a 1 A g⁻¹discharge rate, a power density of 14.4 kW kg⁻¹at a 10 A g⁻¹discharge rate, and a long cycle life critical to energy storage and management. This work demonstrates the application of a new class of stable and tunable redox‐active material for sustainable energy technologies.