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In the past, the two major biomineralization motifs, biosilicification and biocalcification, were considered as two discrete processes. However, there is increasing evidence of the existence of an inextricable relationship between biosilica and calcium-based biominerals.[1] The recent discovery of a unique silica–chitin–aragonite biocomposite in one genus of demosponges (Verongida) introduces a novel mechanism of multiphase hierarchical biomineralization.[2] Considerable effort has been devoted to the development of silica-/calcium-based organic–inorganic hybrids;[3–5] however, none of the techniques used could demonstrate the composite nature of their natural counterparts. Herein, we report a bottom-up, biomimetic biomineralization strategy that results in the intrafibrillar mineralization of collagen with hierarchically arranged silica–apatite multiphase minerals. The mineralization mechanism involves the …