The optimum sample preparation, optical properties, and stability against light and heat for sulfur-perturbed F2+ centers (F2+:S-) in NaCl have been investigated to determine the potential quality as a laser material. F2+:S-’s were introduced into NaCl doped with Na2S by additive coloration and subsequent photoaggregation. Absorption and luminescence bands occurred at 1.18 and 0.832 eV at 80 K, respectively. The excitation spectra for the luminescence showed two maxima at 1.18 and 2.71 eV. The luminescence efficiency was 0.84± 0.03 between 80 and 290 K. Photoexcitation of the F2+ center in F2+:S- to the 2pπu state at 80 K converted the configuration of F2+:S- into the most compact form, and also rotated the F2+ axis by 60°, while the photoexcitation above about 190 K destroyed F2+:S-. F2+:S- was expected to be stable for ∼19 days at 290 K, and ∼400 days at 268 K in the dark.