Europium (Eu)-doped calcium magnesium chlorosilicate [Ca8Mg(SiO4)(4)Cl-2:Eu2+] phosphor particles were prepared by spray pyrolysis and their luminescence characteristics were optimized by changing the Ca precursor type, the Eu2+ content, and the post-treatment temperature. It was found that the ratio of calcium nitrate to calcium chloride, which were used as the source of Ca and Cl, respectively, significantly affects the luminescence intensity and the particle morphology. Photoluminescence intensity was monotonically increased by increasing calcium chloride content with respect to calcium nitrate content in the spray solution due to increases in the crystallinity and phase purity of Ca8Mg(SiO4)(4)Cl-2:Eu2+. Ca8Mg(SiO4)(4)Cl-2:Eu2+ was gradually turned from a spherical shape to a polyhedral shape of micron size as the calcium chloride content was increased in the spray Solution. The concentration quenching of Eu2+ was observed at 0.375 mol % Ca. The optimized CagMg(SiO4)(4)Cl-2: Eu2+, which showed a broad emission spectrum from 460 to 550 mm with a peak position at 502 run. had a high brightness under the excitation by short- and long-wavelength ultraviolet lights and is expected to be Successfully applied as a green phosphor for UV light emitting diodes (LEDs).