An inorganic-organic nanohybrid particle with a two-dimensional chain structure, diphenylsiloxane-silica (Ph 2 SiO-SiO 2 ), was prepared by sol-gel process using diphenyldiethoxysilane (DPDES) and tetraethoxysilane (TEOS), and a high proton conducting polymer of poly(2-acrylamido-2-methyl-1-propane sulfonic acid) (PAMPS) was deposited on the Ph 2 SiO-SiO 2 particles via layer-by-layer assembly. A flexible sheet-like electrolyte was successfully obtained from the resulting PAMPSdeposited particles by pressing. The proton conductivity of the sheet prepared using unmodified Ph 2 SiO-SiO 2 particles was lower than 10 À9 S/cm at 801C. On the other hand, the PAMPSdeposited samples showed proton conductivities B7 orders of magnitude higher than those of the sample prepared using unmodified particles, and their conductivity reached about 1 Â 10 À2 S/cm at 801C and 80% relative humidity. This is ascribed to the PAMPS layer being concentrated at the particle interfaces, which percolated throughout the monolithic sample.