This dataset includes data relating to mesoporous silica films grown from sodium silicate solution precursors: dynamic light scattering (DLS) data for solutions containing cetrimonium bromide and sodium nitrate; small angle X-ray scattering (SAXS) data for films contain cetyltrimethylammonium bromide (CTAB), silica and polyethylenimine (PEI), and silica film; thermogravimetric analysis (TGA) data recording the decomposition of CTAB–PEI–silica in air with temperature; in-situ X-ray reflectivity (XRR) data, surface pressure data, and grazing incidence X-ray scattering (GISAXS) data for the interface between the solution (sodium silicate, CTAB, PEI) and air; and nitrogen sorption data.