Aerosilogel modified with hydroxylaluminum (=Al-OH) groups has been synthesized via the molecular layering procedure, and aerosilogel modified with aminopropylsilyl groups [≡Si(CH₂)₃NH₂] has been prepared via chemisorption of (3-aminopropyl)triethoxysilane. The modified aerosilogel have been further used to prepare composite Nafion-containing electrolytes Nafion. Electrical conductivity of the produced materials has been studied by impedance spectroscopy. Chemical modification of the gel surface strongly affects proton conductivity of Nafion-containing composites.