In situ co-synthesis of nylon 66 (PA66)-silica nanocomposites can be accomplished through solgel chemistry conducted simultaneously with the nylon polymerization. Unfunctionalized silica nanocomposites and bonded silica nanocomposites wherein the inorganic silica phase chemically couples to the nylon polymer through a functionalized silane are generated via the simultaneous initiation of synthesis reactions in the inorganic and organic species. The effects of agitation and water-to-silane molar ratio on the courses of the inorganic and organic reactions and the generated silica morphology in the resulting nanocomposites are investigated using the tools of Brookfield Viscometer, Fourier transform infrared spectroscopy, and transmission electron microscopy. Dynamic mechanical analysis confirms the mechanical reinforcement of the various nanocomposites in relation to their silica content and network morphology. POLYM. ENG. SCI., 2012. (C) 2012 Society of Plastics Engineers