This work successfully verified that the addition of a flux (NH 4 F, NH 4 Cl, and H 3 BO 3 ) during synthesis has an impact on the crystallite size and quantum efficiency of submicron-sized particles of CaMgSi 2 O 6 :Eu 2+ phosphors. The addition of NH 4 F or NH 4 Cl increased the crystallite size in the submicron-sized particles, yielding an increase in emission intensity and quantum efficiency. On the other hand, the use of the H 3 BO 3 flux crystallized a secondary phase, SiO 2 , and changed the lattice parameters, which degraded the luminescent properties. In addition, an excessive amount of NH 4 Cl was examined, resulting in nucleation of a secondary phase, CaSiO 3 , which changed the lattice parameters with no improvement in luminescent properties. These results demonstrate that the addition of a flux could be a method to improve the quantum efficiency of submicron-sized particles composed of nanocrystallites; however, a judicious choice of the flux composition and amount has to be carefully considered.