SrAl2O4:Eu2+,Dy3+ polynary complex nanobelts with long-persisting phosphorescence were synthesized via a facile but efficient combustion method followed by a postannealing reaction at temperature above 900 °C. All the samples emit greenish-yellow light from the d-f transition of Eu2+, and moreover, their wavelength redshifts with increasing calcination temperature since the increase in crystal size and crystalline quality causes a large average optical path and high crystal symmetry, respectively. The decay constant of the sample calcined at low temperature is smaller than that of the one annealed at high temperature owing to the presence of higher densities and depths of electron traps donated by host defects, and the initial brightness of the sample calcined at low temperature is relatively low owing to the small volume fraction from relatively low crystallinity.