Visible-light active, carbon doped and ordered mesoporous SiO₂–TiO₂ nanocomposites (C-OMS@TiO₂-xs) were synthesized from the self-assembly of Si and Ti precursors with block copolymer templates (F127 and P123), hydrothermally treated at 180 °C, and calcination or extraction for removing the templates. XRD patterns and TEM images indicate highly ordered mesopores were formed in C-OMS@TiO₂-xs, and TiO₂ species with a high crystalline degree were homogeneously dispersed into the samples, which formed a stable “brick-and-mortar” nanostructure. N₂ adsorption–desorption isotherms indicate very large BET surface areas (224–553 m² g⁻¹) and pore volumes (0.45–1.4 cm³ g⁻¹) in these samples. EDX spectra and elemental maps further confirm successful doping and homogeneous dispersion of TiO₂ nanocrystals in C-OMS@TiO₂-xs. XPS spectra confirmed the doping of carbon atoms into the lattice of TiO₂ species under high temperature hydrothermal conditions, which results in C-OMS@TiO₂-xs with enhanced visible light response properties, as confirmed by UV-vis diffuse reflectance spectra and photocurrent–time (I–t) curves. Catalytic tests indicate that the synthesized C-OMS@TiO₂-xs show excellent activities for degradation of organic pollutants irradiated with visible light. For instance, degradation of highly concentrated rhodamine B (RhB, 100 ppm) can be completely catalyzed in the water within 50 min. This work provides a facile approach to the targeted synthesis of visible active and ordered mesoporous materials.