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One major challenge of functional material fabrication is combining flexibility, strength, and toughness. In several biological and artificial systems, these desired mechanical properties are achieved by hierarchical architectures and various forms of anisotropy, as found in bones and nacre. Here, it is reported that crystals of Ncapped diphenylalanine, one of the most studied selfassembling systems in nanotechnology, exhibit wellordered packing and diffraction of subÅ resolution, yet display an exceptionally flexible nature. To explore this flexibility, the mechanical properties of individual crystals are evaluated, assisted by density functional theory calculations. Highresolution scanning electron microscopy reveals that the crystals are composed of layered selfassembled structures. The observed combination of strength, toughness, and flexibility can therefore be explained in terms of weak interactions between …