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Titanium dioxide (TiO2) is the most frequently studied semiconducting material for photocatalytic water splitting. One of the favored forms of TiO2 for photocatalytic applications is layers of erected single-crystalline anatase nanosheets (NSs), while the most frequently reported substrate used for its synthesis is a fluorine-doped tin oxide (FTO). Herein we demonstrate that anatase TiO2 NS layers can be similarly grown on a Ta2O5 substrate. We found that a Ta2O5 back contact provides a remarkable improvement of the photocatalytic activ