Mannich‐Type Polymers: A Versatile Platform for Water‐Degradable, Malleable, and Environmentally Responsive Networks

Abstract Polymer waste poses a significant environmental challenge, with current recycling strategies often hindered by inefficient waste collection systems, high production costs, and limited material recyclability. While extensive efforts have been directed toward upcycling or degrading commercial polymers, as well as developing sustainable alternatives, many approaches remain constrained by their reliance on harsh conditions, specialized catalysts, or complex processing methods. In this study, we present a novel strategy to address the challenges by developing mechanically robust polymer networks that are readily degradable in water within 30 days. Our approach leverages a guanidine‐based Mannich‐type reaction utilizing three low‐cost starting materials—guanidine hydrochloride, aldehyde, and diamine—under mild conditions. Unlike traditional thermosets, which are often difficult to recycle, our polymer networks exhibit exceptional processability, enabling the fabrication of various forms, and demonstrate responsiveness to moisture. These properties, coupled with degradability, make them viable candidates for diverse applications. By introducing a scalable and sustainable pathway for designing next‐generation recyclable polymers, our work advances the field of dynamic covalent chemistry and presents a novel class of sustainable polymer networks with significant potential for reducing environmental impact.