Hydrophobic photostable laser dye molecules were incorporated into organically modified silicate matrices by the sol-gel technique. Successful laser oscillation of various pyrromethene dyes doped Ormosil has been achieved. Pumped with a frequency-doubled Q-switch Nd:YAG laser at 532 nm, the laser wavelength is tunable over 44 nm (550~594 nm). A slope efficiency of 61% was obtained from one of the dye-doped Ormosil in the millijoule output energy range. A useful lifetime greater than 2.5×104 pulses at a pump repetition rate of 1 Hz and a pump intensity of 1 J/cm2 was measured, with only a 10% loss in the available output energy.