A wide variety of polymer nanocomposites exhibiting novel property combinat
ions were obtained via in-situ formation of silicate nanofillers during pol
ymerization and processing. Key intermediates were tailor-made silicates wh
ich were rendered organophilic by means of cation exchange and exfoliated u
pon applying shear forces. As a function of organophilic modification, inte
rfacial coupling, and processing conditions it was possible to control nano
structure formation and to improve thermal and mechanical properties such a
s toughness/stiffness balance, heat distortion temperature, and flame retar
dency. Basic structure/property correlations were established for nanocompo
sites based upon in-situ nanofillers and polymers such as polystyrene, poly
amide 12, polypropylene, polymethylmethacrylate, polyurethane, and epoxy re
sins.