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Structural supercapacitors reach high performance with a gradient electrolyte and redox polymer electrodes. 

Ladder-type structures can impart exceptional stability to polymeric electronic materials. This article introduces a new class of conductive polymers featuring a fully ladder-type backbone. A judicious molecular design strategy enables the synthesis of a low-defect ladder polymer, which can be efficiently oxidized and acid-doped to achieve its conductive state. The structural elucidation of this polymer and the characterization of its open-shell nature are facilitated with the assistance of studies on small molecular models. An autonomous robotic system is used to optimize the conductivity of the polymer thin film, achieving over 7 mS cm^−1. Impressively, this polymer demonstrates unparalleled stability in strong acid and under harsh UV-irradiation, significantly surpassing commercial benchmarks like PEDOT:PSS and polyaniline. Moreover, it displays superior durability across numerous redox cycles as the active material in an electrochromic device and as the pseudocapacitive material in a supercapacitor device. This work provides structural design guidance for durable conductive polymers for long-term device operation. 

Photodetectors operating across the near‐ to short‐wave infrared (NIR–SWIR,λ= 0.9–1.8 µm) underpin modern science, technology, and society. Organic photodiodes (OPDs) based on bulk‐heterojunction (BHJ) active layers overcome critical manufacturing and operating drawbacks inherent to crystalline inorganic semiconductors, offering the potential for low‐cost, uncooled, mechanically compliant, and ubiquitous infrared technologies. A constraining feature of these narrow bandgap materials systems is the high noise current under an applied bias, resulting in specific detectivities (D^*, the figure of merit for detector sensitivity) that are too low for practical utilization. Here, this study demonstrates that incorporating wide‐bandgap insulating polymers within the BHJ suppresses noise by diluting the transport and trapping sites as determined using capacitance‐frequency analysis. The resultingD^*of NIR–SWIR OPDs operating from 600–1400 nm under an applied bias of −2 V is improved by two orders of magnitude, from 10⁸to 10¹⁰ Jones (cm Hz^1/2 W⁻¹), when incorporating polysulfone within the blends. This broadly applicable strategy can reduce noise in IR‐OPDs enabling their practical operation and the realization of emerging technologies.