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Organic-inorganic hybrid nano-material has a significant potential for enhancing the charge separation efficiency of photocatalyst. However, it remains an important issue to controllable synthesis new hybrid system with unique structure and earth-abundant materials for boosting photocatalytic hydrogen revolution. We report a facile one-step hydrothermal strategy to fabricate a novel Titania/β-cyclodextrin (TiO 2 /β-CD) organic-inorganic hybrid nano-material with an alveolate structure. In this hybrid system, β-CD not only played a critical role in alveolate structure formation, but also served as a bridge connecting target molecular and active sites on the TiO 2 surface to facilitate the separation and transfer of the photoexcited electrons with prolonged lifetime. As a result, this alveolate TiO 2 /β-CD composite exhibited outstanding photocatalytic activity and a H 2 evolution rate of 725 μmol/g·h was achieved over TiO 2 /β-CD which was 14 times of bare TiO 2 under simulated sunlight. This work paves a way for controllable synthesis of novel organic-inorganic hybrid nano-material with distinct structure for efficient photocatalysis. Image 1 • A novel alveolate organic-inorganic hybrid has been successfully prepared. • The hybrid composite exhibited outstanding photocatalytic activity. • The H 2 evolution rate of TiO 2 /β-CD has a good durability. • This work paves a way for controllable synthesis of organic-inorganic TiO 2. • Limited reports on the photocatalytic water splitting of the TiO 2 /β-CD. [ABSTRACT FROM AUTHOR]