A fundamental limitation of the spectral response of laser-pumped fluorescent nanostructured media was considered in terms of a probabilistic model establishing the relationship between the enhancement factor of a spectral quality and characteristic propagation and amplification scales of pump light and fluorescence in the medium. It was shown that the minimum spectral width of fluorescent response of the pumped medium is limited by competition between the stimulated emission and radiation losses in microscopic fluorescence emitters associated with the speckles randomly modulating the pumping light field. Theoretical results were compared to the experimental data on the spectral properties of the fluorescent response of laser-pumped nanostructured “anatase nanoparticles—dye solutions” systems with various structural and optical properties. Rhodamine 6G and 4-(dicyanomethylene)-2-methyl-6-(p-dimethylaminostyryl)-4H-pyran (DCM) were applied as fluorescent components in the examined systems with various scatter volume fractions, which were pumped by pulse-periodic laser radiation with various intensities at 532 nm. Comparison showed a fair agreement between the theoretical and experimental results.