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We describe a high-modulus toughening mechanism in mature\n                    <jats:italic toggle=\"yes\">Cristaria plicata<\/jats:italic>\n                    nacre arising from a crystalline organic-inorganic framework composed of aragonite nanorods alternately integrated with intratabular biomolecular crystallites. Due to the critical slip-length effect, these crystalline units approach the theoretical limits of modulus and strength. The nanoconfined biomolecular crystallites function as nanopins at interlamellar interphases, alleviating stress concentrations and enabling cross-scale synchronized deformation, thereby conferring high fracture toughness. Inspired by this mechanism, reconstituted nacre fabricated from regenerated aragonite flakes simultaneously achieved high stiffness and crack resistance. 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