This invention is directed to the preparation of neutralized polyelectrolyte complexes exhibiting hydrophobic behavior containing crystals of an organic polycation exchanged lithium and/or sodium water-swelling mica. The process for making such products comprises:(1) forming a glass-ceramic body containing crystals selected from the group of fluorhectorite, hydroxyl hectorite, boron fluorphlogopite, hydroxyl boron phlogopite, and solid solutions among those and between those and other structurally-compatible species selected from the group of talc, fluortalc, polylithionite, fluorpolylithionite, phlogopite, and fluorphlogopite;(2) contacting that body with a polar liquid to cause swelling and disintegration of the body accompanied with the formation of a gel; and(3) contacting said gel with a source of organic polycations to cause a reaction between the Li.sup.+ and/or Na.sup.+ ions from the interlayer of the crystals and to neutralize the charge density of the crystals, thereby forming neutralized polyelectrolyte complex, said organic polycations being selected from the group of(a) a primary amine solubilized with acid,(b) a secondary amine solubilized with acid,(c) a tertiary amine solubilized with acid,(d) a quaternary ammonium acid salt,(e) a quaternary phosphonium acid salt, and(f) a ternary sulfonium acid salt.