In this work, a spray-drying method was used to prepare densely structured Zn2SiO4:Mn phosphor particles. Dextrin as an organic additive was found to play a role in efficiently reducing the hygroscopicity of the metal salts and obtaining dense precursor powders after the drying process. After the heat-treatment process, the dextrin-assisted precursor particles were turned into dense spherically shaped particles with a mean particle size of 1.3 μm and the high crystallinity of a pure Zn2SiO4 phase. The luminescence properties were changed by changing the types of organic additives. The phosphor particles with the smallest surface areaand the powder with the largest crystallite size showed the highest luminescence intensity. Finally, the dense spherical particles obtained from the spray solution containing dextrin had an emission intensity corresponding to 176% that of the phosphor powders prepared from the solution without organic additives.