H +-titanosilicate (H 4Ti 2Si 8O 22 · 4H 2O), formed by proton ion exchange of layered titanosilicate JDF-L1 (Na 4Ti 2Si 8O 22 · 4H 2O) produced intercalation compounds in DDA (dodecylamine)–TEOS (tetraethylorthosilicate) solution. H +-titanosilicate/DDA/TEOS intercalation compounds rapidly hydrolyzed in pure water to form siloxane-pillared H +-titanosilicates. Calcination of siloxane-pillared H +-titanosilicates for 5 h at 500 °C in air resulted in the formation of mesoporous silica-pillared H +-titanosilicate (SPT) derivatives. SPT derivatives exhibited refractions corresponding to a basal spacing of 4.16–4.32 nm, a uniform pore size of 2.8–3.4 nm, and a large surface area of 535–618 m 2/g. The structures and physical properties of SPT derivatives remained stable after heating for 5 h at 700 °C in air. These results indicate that DDA molecules have a decisive role in pore formation within SPT derivatives, because they act as a base catalyst and as a template, like surfactant micelles, during the hydrolysis of TEOS.