Stable blue-green photoluminescent ZnO–SiO2 nanocomposite particles exhibiting quantum efficiency as high as 34.8% under excitation at 360 nm were prepared using a spray-drying process from a feed solution that contained both luminescent ZnO nanoparticles synthesized by a sol–gel method and commercially-available SiO2nanoparticles. The effects of silica nanoparticle size and SiO2-to-ZnO concentration ratio on the PL properties of the composite particles were investigated. The internal structure and chemical composition were investigated in detail using elemental mapping, which revealed that ZnO nanoparticles were well-dispersed within silica nanoparticle matrix. At a LiOH concentration of 0.23 M, the predicted ZnO crystallite diameter before and after spray drying was approximately constant at 3.3 and 3.6 nm, respectively. This result indicates that ZnO particle growth was inhibited and therefore the PL property of ZnO nanoparticles was stably preserved in the composite.