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This study proposes a strategy based on heterovalent ion doping that gives rise to a synergistic piezo‐phototronic effect with significantly improved catalytic activity and leads to selective catalytic enhancement for specific pollutants. Owing to the enhanced light absorption, hydrogen evolution rates are as high as 3704 and 3178 µmolg−1 h−1 in 0.01Li‐doped BaTiO3 and 0.02La‐doped BaTiO3 nanosheets,...