Calcium aluminate phosphor co‐doped Eu2+, Dy3+, Nd3+ is prepared by the combustion method. We study systemically the influences of the quantity of mixed Dy3+ ion, the quantity of flux H3BO3, the differences in dispersing methods between magnetic stirring and ultrasonic dispersing and the combustion temperature on the long‐persistence phosphor. The analytical results indicate that Dy3+ ion improves the properties of the phosphors CaAl2O4:Eu2+, Nd3+. The appropriate quantity of flux H3BO3 to reduce the forming temperature of the sample was determined. The monoclinic single phase of CaAl2O4 formed at 500°C and remained steady. The calcium aluminate co‐doped Eu2+, Dy3+, Nd3+ was synthesized by dispersal of the raw material using the ultrasonic method, and it had better optical properties. Copyright © 2009 John Wiley & Sons, Ltd.