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In this study, 2D/3D TiO2/ZnIn2S4 nanostructures with TiO2 sheet cluster embedded into ZnIn2S4 micro flowers were fabricated via hydrothermal method. The matched band structure, the enlarged surface area and the efficient photo-induced charge transfer offered by effective heterostructures formed between the two components endowed the TiO2/ZnIn2S4 nanoarchitecture with excellent photocatalytic Cr(VI) reduction and tetracycline hydrochloride (TC) degradation performance. Especially, the Cr(VI) photoreduction efficiency of 50% TiO2/ZnIn2S4 was 8.8 times higher compared to pure ZnIn2S4. The enhanced separation efficiency of photo-excited charge carriers was induced by the matched band structure, the enlarged surface area and the strong interaction between TiO2 and ZnIn2S4. The key roles of ·O2− was confirmed via trapping experiments. Otherwise, the pathway of TC degradation was investigated. The proposed mechanism during photocatalysis process was also discussed according to the photocatalytic and characterization results.