Natural materials such as bone, tooth, and nacre are nanocomposites of proteins and minerals with superior strength. Why is the nanometer scale so important to such materials? Can we learn from this to produce superior nanomaterials in the laboratory? These questions motivate the present study where we show that the nanocomposites in nature exhibit a generic mechanical structure in which the nanometer size of mineral particles is selected to ensure optimum strength and maximum tolerance of flaws (robustness). We further show that the widely used engineering concept of stress concentration at flaws is no longer valid for nanomaterial design.

Silk fibroin, a natural multi-domain protein, has attracted great attention due to its superior mechanical properties such as ultra-high strength and stretchability, biocompatibility, as well as its versatile biodegradability and processability. It is mainly composed of β-sheet crystallites and amorphous domains. Although its strength is well known to be controlled by the dissociation of protein chains from β-sheet crystallites, the way that water as the solvent affects its strength and the reason that its theoretically predicted strength is several times higher than experimental measurement remain unclear. We perform all-atom molecular dynamics simulations on a β-sheet crystallite of Bombyx mori silk. We find that water solvent reduces the number and strength of hydrogen bonds between β-chains, and thus greatly weakens the strength of silk fibroin. By dissociating protein chains at different locations from the crystallite, we also find that the pulling strength for the interior chains is several times higher than that for the surface/corner chains, with the former being consistent with the theoretically predicted value, while the latter on par with the experimental value. It is shown that the weakest rupture strength controls the failure strength of silk fibre. Hence, this work sheds light on the role of water in the strength of silk fibroin and also provides clues on the origin of the strength difference between theory and experiment.

Biological nanocomposites, such as bone, tooth, shell, and wood, exhibit exceptional mechanical properties. Much recent effort has been directed at exploring the basic mechanical principles behind the microstructures of these natural materials to provide guidelines for the development of novel man-made nanocomposites. This article reviews some of the recent studies on mechanical properties of biological nanocomposites, including their stiffness, strength, toughness, interface properties, and elastic stability. The discussion is focused on the mechanical principles of biological nanocomposites, including the generic nanostructure of hard-mineral crystals embedded in a soft protein matrix, the flaw-tolerant design of the hard phase, the role of the soft matrix, the hybrid interface between protein and mineral, and the structural hierarchy. The review concludes with some discussion of and outlook on the development of biomimicking synthetic materials guided by the principles found in biological nanocomposites.