Combination of supramolecular chemistry with molecular recognition has been successfully applied to creating large superstructures with a wide variety of morphologies. Control of shapes and patterns of ordered molecular assemblies in nano and micro scales has attracted considerable interest as promising bottom-up technology. It is known, however, that these molecular assembling superstructures are fragile, reflecting the characteristic of the non-covalent interaction, a driving force operating in these molecular systems. In fact, they easily collapse or change by small perturbation in the environmental conditions. Thus, over the last decade, researchers have been seeking possible methods for the immobilization these superstructures. This critical review focuses on recent advances in in situ post-modification under the influence of the molecular assemblies as templates and polymerization of ordered molecular assemblies such as organogel fibers and crystals to preserve their original superstructures and intensify their mechanical strength.