SrAl2O4:Eu2+ phosphor crystals co-doped with auxiliary activators such as La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, or Y have been grown by the floating zone (FZ) technique. Photoluminescence spectrum (PL), time-resolved PL, and thermally stimulated luminescence (TSL) are evaluated to clarify the long-duration phosphorescence mechanism of SrAl2O4, Eu, and Ln phosphors. TSL spectra were measured in the temperature range from RT to 600 K to evaluate the depth and densities of the traps generated by the doping of auxiliary activators that are responsible for the long-duration phosphorescence. The peak wavelength of PL does not vary with auxiliary activator elements, while decay curves vary greatly with the auxiliary activators. The trap depth and the densities of the trapped carriers estimated based on the hole trap model also vary with the auxiliary activator elements. The traps generated at around E = 0.5 eV by the auxiliary activators, Nd, Dy, and Tm, with sufficient densities are effective for the long-duration phosphorescence.