Phosphor material CaAl2O4:Eu2+codoped with varying concentrations ofNd3+was prepared by solid-state reaction method. Prepared materials with 1 mol%Eu2+andNd3+(0.5 to 5 mol%) show high brightness and long persistent luminescence. The phase and crystallinity of the synthesized materials were investigated by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). Photoluminescence excitation and emission spectra were taken to investigate the luminescence characteristics. Broadband UV excited luminescence of the CaAl2O4:Eu2+,Nd3+was observed in the blue region (λmax= 440 nm) due to transitions from4f 6 5d1to the4f 7configuration of theEu2+ion. TheNd3+ion doping in the phosphor generates deep traps which result in long afterglow phosphorescence.