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In this study, TiO2 nanocrystals were synthesized in the scaffold of cellulose nanocrystal (CNC) using in situ hydrolysis, where the morphology and size of TiO2 was controlled by CNC's functional groups and surface charge. The resulting TiO2/CNC nanocomposites showed a superior photocatalytic activity for Cr(VI) reduction under visible light (λ 420 nm) due to the combined effects of small TiO2 size and ligand-to-metal charge transfer (LMCT) complex between CNC and TiO2. It was found that the charge-enriched CNC not only acted as a template to direct th