Nerita undata is a marine gastropod, the shell of which consists of an external layer composed of very fine, long and undulating calcite prisms, and of an internal aragonite crossed-lamellar layer. As for any Ca-carbonate shell, both layers are composite materials, resulting from the sub-micrometric association of organic macromolecules with the mineral phase. But at the transition between the two layers, in situ synchrotron-based mapping using µ-XANES spectroscopy performed at the S K-edge and SR-FTIR spectroscopy reveals that biochemical compositions change correlatively with the mineral phase, such as displayed by the distribution of sulfur-containing organic compounds (S-polysaccharides or S-amino acids) and organic molecular groups (amide I and II bands). These results highlight the complex change of secretory activity operated by the mineralizing tissue (the mollusk mantle) between these two parts of the shell, which is suspected to minutely control the setting-up of the crossed-lamellar microstructural pattern over the calcite prisms-A not so straightforward feature.