High‐Performance Organic Aerogels Tailored for Versatile Recycling Approaches: Recycling‐Reforming‐Upcycling

Abstract Organic aerogels are emerging as promising materials due to their versatile properties, rendering them excellent candidates for a variety of applications in the fields of thermal insulation, energy storage, pharmaceuticals, chemical adsorption, and catalysis. However, current aerogel designs rely on cross‐linked polymer networks, which lack efficient end‐of‐use solutions, thereby hindering their overall sustainability. In this study, a facile synthesis of organic aerogels with a unique combination of imine and cyanurate moieties is presented, resulting in high‐performance, lightweight insulating materials. The aerogels’ structure, ensures mechanical robustness, thermal resistance, and hydrophobicity without additional treatments, crucial for long‐term performance. Additionally, in response to the currently unsustainable use of cross‐linked polymer materials, the molecular design offers diverse avenues of chemical recycling. These include full depolymerization back into the original monomers, partial network fragmentation producing soluble oligomers that can be promptly employed to fabricate new aerogels, and upcycling of aerogel waste into useful building blocks. This work pioneers a novel approach to material design, emphasizing recyclability as a core feature while maintaining high‐performance excellence.