In this study, we examined the potential for perylene dye doped nanoparticles to enhance Light Emitting Diodes (LED) efficacy by minimizing pi-pi intermolecular aggregation, and enhancing photoluminescence and photostability of the dye molecules in the solid state. Towards this end, we encapsulated perylene dyes, suitably modified with a reactive silica precursor, into silica nanoparticles within a silica-dye silica concentric layered shell. We found that the fluorescent yield was higher when the dye was embedded in a buried concentric shell within the silica nanoparticles (NPs) compared to an undoped shell/dye doped core nanoparticle morphology or unencapsulated dye with the same net dye concentration in solution. A strong dependence of relative quantum yield on dye doping concentration in the silica-dye-silica nanoparticles was observed. The uniform similar to 100 nm large silica-dye-silica layered nanoparticles were used to prepare transparent dye doped silica nanoparticle/silicone nanocomposites. Dye doped silica nanoparticle/silicone-nanocomposites exhibited higher photostability than the unencapsulated dye samples during long time aging tests under a blue LED with a wavelength of 455 nm at 300 +/- 3% mA for 24 h. Novel dye doped layered silica NPs and their nanocomposites offer scope for developing organic luminescent materials into efficient and color-tunable light emitters for low-cost display, lighting, and optical communication applications. (C) 2019 Elsevier Inc. All rights reserved.