Carbon/silica (carbosil) samples prepared utilizing mesoporous silica gel (Si-60) modified by methylene chloride pyrolysis were studied by nitrogen adsorption, quasi-isothermal thermogravimetry, p-nitrophenol adsorption from aqueous solution, and H-1 NMR methods. The structural characteristics and other properties of carbosils depend markedly on the synthetic conditions and the amount of carbon deposited. The changes in the pore size distribution with increasing carbon concentration suggest grafting of carbon mainly in pores, leading to diminution of the mesopore radii. However, heating pure silica gel at the pyrolysis temperature of 550 degrees C leads to an increase in the pore radii. The quasi-isothermal thermogravimetry and H-1 NMR spectroscopy methods used to investigate the water layers on carbosils showed a significant capability of carbosils to adsorb water despite a relatively large content of the hydrophobic carbon deposit, which represents a nonuniform layer incompletely covering the oxide surface.