The preparation and characterization of new organic/inorganic composites by the consecutive adsorption of weak polyelectrolytes on silica particles were studied in the article. Two polycations containing primary amine groups in the side chains, poly(vinylamine) or poly[N(beta-aminoethylene) acrylamide], and poly(acrylic acid) as polyanion were used for the hybrid materials construction. The stability of the organic/inorganic composites has been increased by a heat-induced reaction at 150 A degrees C. The organic/silica hybrids properties were monitored by potentiometric titration, laser light scattering, infrared spectroscopy, and thermogravimetric analysis. The adsorption of methylene blue by the composite materials has been tested. The dye adsorption capacity was strongly influenced by the dye concentration, the nature of the last adsorbed layer, the polyions concentration, and the composite thermal treatment.