Highly crystalline TiO nanostructured films were synthesized by a simple steam treatment of a TiCl precursor film under a saturated water vapor atmosphere at 125 °C, here referred to as the steam-annealing method. In a single TiO film preparation step, a bilayer structure comprising a compact bottom layer and a mesoporous surface layer was formed. The mesoporous layer was occupied by bipyramidal nanoparticles, with a composite phase of anatase and brookite crystals. Despite the low-temperature treatment process, the crystallinity of the TiO film was high, comparable with that of the TiO film sintered at 500 °C. The compact double-layered TiO film was applied to perovskite solar cells (PSCs) as an electron-collecting layer. The PSC exhibited a maximum power conversion efficiency (PCE) of 18.9% with an open-circuit voltage ( V) of 1.15 V. The PCE and V were higher than those of PSCs using a TiO film formed by 500 °C sintering.
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