A triple-layer TiO2 (TiO2-TL) structure was synthesized with an over-layer composed of TiO2 flower-like microspheres (MSs), a middle layer of nanosheet arrays (NSAs) and an under-layer of compact film (CF) on a titanium (Ti) mesh substrate using a one-step hydrothermal route and used to make a series of flexible dye-sensitized solar cells (DSSCs).