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In sharp contrast to conventional photosensitization methods in which the organic pigments were often adsorbed, herein we present a study on natural vegetable pigment inserted TiO₂ aerogel nanocomposites and we directly use red cabbage anthocyanin (RCP) as a structure-directing agent. It was found that pure TiO₂ aerogel nanocomposite did not exhibit any meaningful activity for photocatalytic reduction of Cr(VI). However, the photocatalytic reduction activity was greatly improved by the RCP inserted TiO₂ aerogel nanocomposites under visible-light irradiation, which was approximately 2- and 12.3-fold higher than that of TiO₂ aerogel conventionally photosensitized by RCP and pure TiO₂ aerogel nanocomposites, respectively. It also exhibited good stability and could be reused at least three times without losing a significant amount of its activity.