Aerogels with abundant nanopores and large specific surface areas have extensive potential in various applications but are constrained by fragility and difficulty in degradation. Currently, the exploration of adaptive and reprocessing aerogels has become increasingly urgent, as the demand for intelligent and sustainable materials intensifies. Here, we present a molecular weaving strategy to construct molecularly woven polymer aerogels (WPAs) via catalyst-free aldimine condensation between prewoven aldehyde-functionalized Cu(I) bisphenanthroline (Cu(PBD)