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Highly fluorescent nanocoils and nanotubes were assembled from elaborately designed asymmetric perylene diimide (PDI) molecules. These nanomaterials exhibited unprecedented sensitivity to trace amines, even three orders of magnitude greater than previously reported solid nanofibers. The coiled and tubular nanostructures as new sensing materials offer a novel option for optimizing the sensitivities of fluorescence sensors based on organic nanomaterials.