Low-cost controllable solution-based processes for preparation of titanium oxide (TiO 2) thin films are highly desirable, because of many important applications of this oxide in catalytic decomposition of volatile organic compounds, advanced oxidation processes for wastewater and bactericidal treatments, self-cleaning window glass for green intelligent buildings, dye-sensitized solar cells, solid-state semiconductor metal-oxide solar cells, self-cleaning glass for photovoltaic devices, and general heterogeneous photocatalysis for fine chemicals etc. In this work, we develop a solution-based adsorptive self-assembly approach to fabricate anatase TiO 2 thin films on different glass substrates such as simple plane glass and patterned glass at variable compositions (normal soda lime glass or solar-grade borofloat glass). By tuning the number of process cycles (i.e., adsorption-then-heating) of TiO 2 colloidal suspension, we could facilely prepare large-area TiO 2 films at a desired thickness and with uniform crystallite morphology. Moreover, our as-prepared nanostructured TiO 2 thin films on glass substrates do not cause deterioration in optical transmission of glass; instead, they improve optical performance of commercial solar cells over a wide range of incident angles of light. Our as-prepared anatase TiO 2 thin films also display superhydrophilicity and excellent photocatalytic activity for self-cleaning application. For example, our investigation of photocatalytic degradation of methyl orange indicates that these thin films are indeed highly effective, in comparison to other commercial TiO 2 thin films under identical testing conditions. © 2012 American Chemical Society.