Mixed amphiphilic block copolymers of poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide) (PEO-PPO-PEO) and polydimethylsiloxane-poly(ethylene oxide) (PDMS-PEO) have been successfully used as co-templates to prepare ordered mesoporous polymer-silica and carbon-silica nanocomposites by using phenolic resol polymer as a carbon precursor via the strategy of evaporation-induced self-assembly (EISA). The ordered mesoporous materials of 2-D hexagonal (p6m) mesostructures have been achieved, as confirmed by small-angle X-ray scattering (SAXS), transmission electron microscopy (TEM), and nitrogen-sorption measurements. Experiments show that using PDMS-PEO as co-template can enlarge the pore sizes and reduce the framework shrinkage of the materials without evident effect on the specific surface areas. Ordered mesoporous carbons can then be obtained with large pore sizes of 6.7 nm, pore volumes of 0.52 cm(3)/g, and high surface areas of 578 m(2)/g. The mixed micelles formed between the hydrophobic PDMS groups and the PPO chains of the F127 molecules should be responsible for the variation of the pore sizes of the resulting mesoporous materials. Through the study of characteristics of mesoporous carbon and mesoporous silica derived from mother carbon-silica nanocomposites, we think mesoporous carbon-silica nanocomposites with the silica-coating mesostructure can be formed after the pyrolysis of the PDMS-PEO diblock copolymer during surfactant removal process. Such method can be thought as the combination of surfactant removal and silica incorporation into one-step. This simple one-pot route provides a pathway for large-scale convenient synthesis of ordered mesostructured nanocomposite materials.