A layer-by-layer (LBL) assembly technique was used to prepare a nanostructured analogue of nacre from inorganic nanometer-sized sheets of Na+-Montmorillonite clay (C) and a polyelectrolyte, poly(diallyldimethylammonium chloride)(PDDA). LBL technique has been found to be applicable for the preparation of superhydrophobic surfaces, 311 sensors and semipermeable membranes and biomolecules delivery, optically active and responsive films,fuel cells and photovoltaic materials, bioresponsive coatings, and magnetic devices. Using the mix-and-match approach to LBL films, that is, stratified multilayers, the mechanical properties can be incorporated in virtually any LBL functionality, if a convenient pair of LBL partners is available. It was observed that DOPA (L-3,4-dihydroxyphenylalanine) molecules impart unusual adhesive strength to the clay composite and the hardening mechanism found in the natural cement.