SrAl2O4:Eu green phosphor was prepared by spray pyrolysis and its luminescence properties were controlled by replacing the Al sites with boron and using organic modifier or drying control chemical additive. It was clear that the substitution of B into the Al sites was helpful to obtain pure monoclinic SrAl2O4 phase and greatly enhance the emission intensity. In terms of the emission intensity, the optimal content of boron was about 1 at% with respect to the aluminum element. The luminescence intensity of Sr0.9Al1.98B0.02O4:Eu0.1 phosphor could be improved by the use of 0.2 M organic additives in the spray solution. Futhermore, using 0.5 M dimethylformamide(DMF) as a drying control chemical with organic additives made it possible to improve about 172% the emission intensity of Sr0.9Al1.98B0.02O4:Eu0.1 phosphor. According to XRD analysis, the organic additive and DMF used enhanced the crystallinity without any change in the crystal phase. When used only the organic additive without DMF, the surface area of the prepared Sr0.9Al1.98B0.02O4:Eu0.1 phosphor became enlarged. The use of DMF with the organic additive resulted in significant reduction in the surface area. It was concluded that the increase of the crystallinity as well as the reduction of surface area mainly contribute to the improvement in the luminescence intensity of Sr0.9Al1.98B0.02O4:Eu0.1 phosphor prepared using DMF and organic additives.