Anisotropic ZnS Nanoclusters/Ordered Macro‐Microporous Carbon Superstructure for Fibrous Supercapacitor toward Commercial‐Level Energy Density

Abstract Fibrous supercapacitor (FSC) is of great attention in wearable electronics, but is challenged by low energy density, owing to disordered diffusion pathway and sluggish redox kinetics. Herein, using micro‐reaction strategy, an anisotropic superstructure is developed by in situ anchoring ultrafine zinc sulfine (ZnS) nanoclusters on conductively ordered macro‐microporous carbon skeleton via interfacial CSZn bonds (ZnS/SOM‐C). The anisotropic superstructure affords 3D ordered macro‐microporous pathways, large accessible surfaces, and highly dispersed active sites, which exhibit enhanced electrolyte mass diffusion, rapid interfacial charge transfer, and large faradaic ions storage (capacitance of 1158 F g⁻¹ in KOH aqueous solution). By microfluidic spinning, the ZnS/SOM‐C is further assembled into fibrous electrode of FSC that delivers high capacitance (791 F g⁻¹), commercial‐level energy density (172 mWh g⁻¹), and durable stability. As a result, the FSC can realize wearable self‐powered applications (e.g., self‐cleaning ventilatory mask, smartwatch, and display), exhibiting the superiority in new energy and wearable industry.