Nd3+-ion-doped ZnCl2-based glasses were prepared via the melt-quenching method. The Nd3+-ion upconversion excitation mechanism and the ability to disperse Nd3+-ions into ZnCl2-based glasses were investigated using absorption and upconversion fluorescence spectra of Nd3+ ions. The ZnCl,based glass that had an average cationic radius equal to the ionic radius of Nd3+ (98 pm) had the greatest ability to disperse Nd3+ ions. The 20KCl-25BaCl(2).55ZnCl(2) glass, which had the average cationic radius nearest to 98 pm, dispersed Nd3+ ions the most, and it had the strongest upconversion fluorescence.