We report on the synthesis, characterization, and physical properties of modified polymeric matrices incorporating silicon atoms in their structure and doped with laser dyes. When the silicon-modified organic matrices incorporated pyrromethene 567 (PM567) and pyrromethene 597 (PM597) dyes as actual solid solutions, highly photostable laser operation with reasonable, nonoptimized efficiencies was obtained under transversal pumping at 532 nm. At a pump repetition rate of 10 Hz, the intensity of the laser emission remained at the level or above the initial lasing intensity after 100 000 pump pulses in the same position of the sample, corresponding to an estimated accumulated pump energy absorbed by the system of 518 and 1295 GJ/mol for PM567 and PM597, respectively. When the pump repetition rate was increased to 30 Hz, the laser emission of dye PM567 decreased steadily and the output energy fell to one-half its initial value after an accumulated pump energy of 989 GJ/mol. Dye PM597 demonstrated a remarkable photostability, and under 30 Hz pumping the laser emission from some samples remained stable after 700 000 pump pulses in the same position of the sample, corresponding to an accumulated pump energy of 17 300 GJ/mol. Narrow linewidth operation with tuning ranges of up to 31 nm was obtained with both pyrromethene dyes when some of the samples were incorporated into a grazing-incidence grating oscillator.