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One of the interesting characteristics of biominerals is that they often incorporate a biomacromolecular matrix while still diffracting X-rays or electron beams as single crystals.This unique combination of composite structure and single-crystallinity inspires a novel approach to functionalize single crystals by incorporating additives inside.Here,we examine,in detail,the internal structure of synthetic calcite crystals grown in an agarose hydrogel and show that the gel-grown calcite crystals,like biogenic calcite crystals,incorporate the polymer network without disrupting their single crystal nature.