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Abstract While various plastic waste management practices are demonstrated to result in materials with similar properties, morphological features of plastic waste are often lost after recycling/upcycling. Particularly, synthetic textiles are a severely underutilized waste stream that contains built‐in value stemming from their woven architectures. This work demonstrates a simple upcycling strategy to convert polypropylene‐based (PP) woven fabrics to carbon fiber mats through direct pyrolysis for direct use in various end applications without need of additional processing steps, distinct from prior works converting plastic waste to carbon‐based additives. The retention of material properties and architectures, taking advantage of the inherent value with initial product manufacturing, is investigated, with optimal conditions resulting in consistent high carbon yields. Moreover, the textile‐derived carbon shows exceptional Joule heating performance, which can be employed in various heating applications, resulting in reduced energy consumption compared to conventional heating. Furthermore, decoration of fabric‐derived carbon with metal nanoparticles is demonstrated through electroplating, leading to altered surface functionality and further enhanced Joule heating performance. This work introduces a scalable method for upcycling of plastic waste to functional carbons that can completely retain initial material architectures with controlled shrinkage, providing a viable strategy for generating value‐added products toward electrification of heating processes. 

Abstract Electrified thermal chemical synthesis plays a critical role in reducing energy consumption and enabling the industrial decarbonization. While Joule heating offers a promising alternative to gas‐burning furnace systems by directly heating substrates via renewable energy supply, most approaches can only heat the reactor, not the catalytic sites. This limitation stems from the lack of methods to on‐demand create Joule heaters containing in situ loaded catalytic nanoparticles. This work introduces a scalable platform for producing carbonaceous Joule heaters embedded with catalytic nanoparticles from 3D‐printed polypropylene precursors, prepared through crosslinking, metal nitration immersion, and pyrolysis steps. Specifically, sulfonate groups on crosslinked PP can bind with metal ions, yielding well‐dispersed, nanosized particles within a carbon structure that maintains macroscopic dimensional accuracy throughout the manufacturing. The approach is modular, allowing control over particle size and composition. Structured carbon with in situ loaded nickel nanoparticles demonstrates efficient Joule heating, high catalytic activity, and significantly reduced activation energy for catalytic ammonia decomposition. This work provides an innovative material and manufacturing platform to produce structured, catalytically active Joule heaters for decarbonization of chemical synthesis and energy production.