A promising strategy to design highly active catalysts is to use multicomponent catalysts including active metals (such as platinoids) and organosilica as a substrate. In this article, we develop stable OrganoSilica Sandwiches (OSS) consisting of sandwiched metallic layers between organosilica layers. The formation of such a sandwich-like organosilica@platinoid@organosilica material was obtained from bis-silica-alkylammonium carbamate dimers, acting as a template for the immobilization of platinoid salt complexes or metallic nanoparticles in the interlayer space after a reduction treatment. The layered templates and the sandwich structures were investigated by small angle X-ray scattering, coupled thermogravimetric analysis and mass spectrometry, and Raman spectroscopy. It was demonstrated that the meso-structure of the initial template material is not affected by the chemical steps involved in the synthesis of the material and does not depend on the incorporated metal.