Coesite nanocrystals have been synthesized from periodic mesoporous organosilica (PMO) with (CH2)2 bridges heated at 300 °C for 150 min and 12 GPa. The crystals are not sintered, single crystalline, and have diameters of ca. 100–300 nm. Below 300 °C, an amorphous non-porous organosilica glass was obtained. Heating above 300 °C at 12 GPa results in the rapid crystal growth and micron size coesite crystals were formed.