The present paper gives a brief account of the latest advances in understanding of the mechanism and implications of dye adsorption with a special focus on layered silicate surfaces. It has been clearly demonstrated that the controlled adsorption of novel or already well-known dyes has equally great yet unexplored potential. In principle, the well-engineered surface confinement of the molecules may lead to their aggregation, adsorption, or intercalation-induced fluorescence emission even with conventional dyes, which are not considered as luminophores in solutions or in the solid state. We envision the utilization of silicate-based heterogeneous systems to produce novel polymer blended films or structured liquids, as well as to develop a plethora of other photophysical and biomedical applications.