Phosphor nanoparticles (e.g., SrTiO3:Pr,Al and (Y,Gd)3Al5O12:Ce) were prepared using a conventional spray pyrolysis method in conjunction with a polymer-assisted heat treatment (annealing). The effects of spray/annealing temperatures, polymer type, polymer concentration, and salt addition on the morphology, crystallinity, particle/crystal size, and the photoluminescence intensity of as-prepared as well as annealed phosphor particles were investigated. The results showed that the nanocrystal growth of as-prepared-sprayed submicrometer particles was improved and that the nanocrystal networks disintegrate into nanoparticles when polymer or salt solutions are added during the heat-treatment process. The additional combustion heat and gas evolution during the thermal reaction of polymer appear to be the main reasons for this. On the contrary, only compacted agglomerated particles rather than dispersed nanoparticles were found in the case of annealing without polymer/salt addition.