A room temperature based environmentally friendly aqueous solution synthesis route was developed to fabricate highly dispersed small SnO2 nanoparticles (3-5 nm) without the application of any pressurized reaction vessel or organic solvents. The subsequent treatments, that is, dialyzing and freezing, allow for the acquision of dual-function nanostructures with sheet-like feature and large aspect ratio except for the ordinary irregular aggregates. Dye-sensitized solar cells (DSCs) constructed with the resultant multifunctional SnO2 showed an outstanding photovoltaic conversion efficiency (PCE) of 6.92% and an unexpected JSC of 19.5 mA cm-2 at an optimized thickness of 14.1 μm. The excellent performance can be ascribed to the effective coordination of the favorable features (i.e., strong light scattering, large dye loading capability, and fast electron transport) via rational film thickness control as indicated by diffused reflectance spectra, UV-vis absorption spectra, and electrochemical impedance spectroscopy (EIS). [ABSTRACT FROM AUTHOR]