Plasticized and Crystallized Bio‐Electrode for Sustainable Electronics

Abstract The accelerated iteration of electronic products has triggered an unprecedented e‐waste crisis, posing serious environmental challenges to conventional material disposal strategies. In response to this dilemma, there is a pressing need for sustainable electronic materials that combine desired performance with environmental recyclability. Here, a glycerol‐plasticized, PEDOT‐crystallized, and closed‐loop recyclable cellulose‐based conductive film is developed for sustainable electronics. Carboxylated carbon nanotubes (CCNTs) are embedded into a TEMPO‐oxidized cellulose nanofibers (TOCNF) matrix to form a primary conductive framework, further reinforced by poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) bridging. A subsequent glycerol treatment imparts dual effects—plasticizing the cellulose network for enhanced flexibility and inducing PEDOT crystallization for improved charge transport. The resulting film exhibits balanced flexibility, stable conductivity, recyclability, and reliable performance in real‐time electromyography (EMG) sensing. This work offers a promising strategy for next‐generation skin‐interfaced bioelectronics, addressing the urgent need for circular materials in the era of electronic overproduction.