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Supramolecular self-assembly is an increasingly popular approach to design and prepare functional materials, for various applications such as organic electronics and sensing. Despite allowing for a precise organization of photo- and electro-active building blocks, supramolecular assemblies often show poor kinetic stability, which limits their application. Among the recent strategies developed to circumvent this issue, the covalent stabilization of supramolecular self-assembly with polydiacetylene moieties is a particularly attractive approach to well-defined nanomaterials. In this review, we present the most recent examples of covalent rigidification of supramolecualr self-assemblies through the photopolymerization of diacetylene moieties. This approach has not only shown great promise for the stabilization of supramolecular assemblies through covalent bond formation, but also showed great promise for the rational …