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Biological structural composites such as bones, teeth and mollusc shells exhibit unique architectures that find few counterparts among man‐made materials. Combining the rich chemistry of synthetic systems with the intricate structural design principles of biological composites should lead to materials exhibiting unprecedented properties. In this chapter, we briefly discuss some of these natural design principles and present recent attempts to apply them in synthetic systems using engineered processing routes. Although these synthetic processing methods greatly differ from the biomineralization processes undertaken by living organisms, several have proven effective in assembling structures that replicate some of nature's design principles. The examples presented here are meant to illustrate the enormous potential a bio‐inspired approach has towards the development of enhanced and unusual synthetic composites.

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