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Living organisms have ingeniously evolved functional gradients and heterogeneities to create high-performance biological materials from a fairly limited choice of elements and compounds during long-term evolution and selection. The translation of such design motifs into synthetic materials offers a spectrum of feasible pathways towards unprecedented properties and functionalities that are favorable for practical uses in a variety of engineering and medical fields. Here, we review the basic design forms and principles of naturally-occurring gradients in biological materials and discuss the functions and benefits that they confer to organisms. These gradients are fundamentally associated with the variations in local chemical compositions/constituents and structural characteristics involved in the arrangement, distribution, dimensions and orientations of the building units. The associated interfaces in biological materials …