Rutile TiO2 particles made by flame spray pyrolysis (FSP) were coated in a single step with SiO2 layers in an enclosed flame reactor. This in situ particle coating was accomplished by a hollow ring delivering hexamethyldisiloxane (HMDSO) vapor (precursor to SiO2) through multiple jets in swirl cross-flow to Al-doped nanostructured rutile TiO2 aerosol freshly made by FSP of a solution of titanium tetraisopropoxide and aluminum sec-butoxide in xylene. The as-prepared powders were characterized by (scanning) transmission electron microscopy (STEM and TEM), energy dispersive X-ray analysis, X-ray diffraction, nitrogen adsorption, electrophoretic mobility, DC plasma optical emission (DCP-OES), and Fourier transform infrared (FT-IR) spectroscopy. The coating quality was assessed further by the photocatalytic oxidation of isopropyl alcohol to acetone. The effect of HMDSO injection point and vapor concentration on product particle morphology was investigated. The titania particles were uniformly SiO2-coated with controlled and uniform thickness at a production rate of about 30 g h(-1) and exhibited limited, if any, photoactivity. In contrast, spraying and combusting equivalent mixtures of the above Si/Al/Ti precursors in the above reactor (without delivering HMDSO through the hollow ring) resulted in particles segregated in amorphous (SiO2) and crystalline (TiO2) domains which exhibited high photocatalytic activity.