Organic-inorganic nano-materials have attracted growing attention due to their potential applications for optoelectronic devices, sensors, and heterogeneous catalysts. We reported here on the preparation of polynary nanocomposites composed of poly(4-vinylpyridine) (P4VP) functionalized multi-walled carbon nanotubes (MWNTP4VP), silica nanoparticles (nano-SiO 2), viologens, and/or phosphomolybdic acid (PMA), in which the MWNTP4VP, nano-SiO 2 , and viologens were covalently connected while PMA was electrostatically adsorbed. Thermogravimetric analysis revealed that the nanocomposites were composed of about 40-45% MWNTs, 40-45% nanoSiO 2 , as well as 10-15% organic species and others. The preparation processes and compositions of the nanocomposites were characterized using Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. Field emission transmission electron microscopic images revealed that the nano-SiO 2 BenV particles were strongly attached