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ZnIn2S4 is a promising candidate for photocatalysis. However, it is still facing great challenge to improve its photocatalytic activity through rationally regulating its microstructures. Herein, ZnIn2S4 micro-flowers with different self-assembly microstructures were synthesized by solvent induced through one-step hydrothermal method, and were used as catalytic dehydrogenation of 1,2,3,4-tetrahydroisoquinoline to 3,4-dihydroisoquinolines. Different solvents have great effects on the microstructure of ZnIn2S4. The surface of ZIS-H2O petals is relatively smooth, and the petals of ZIS-EtOH are micro-discoid and relatively rough. The microstructure of ZIS-EG is the smallest and consists of countless irregular thin nanosheet. The results show that ZIS-EG assembled with ethylene glycol as solvent has the best photocatalytic activity in the catalytic dehydrogenation. The maximum conversion of 98% as well as the selectivity of 99% of 3,4-dihydroisoquinolines was accomplished under air condition with 7-h visible-light irradiation. The excellent photocatalytic activity of ZIS-EG benefits from its excellent absorption of visible light as well as the separation efficiency of photogenerated carriers. Therefore, this work has provided an effectively method to accelerate the photocatalytic activity through solvent-induced controlling microstructures. A series of ZnIn2S4 photocatalysts with different microscopic morphologies were synthesized, and were used as catalytic dehydrogenation of 1, 2, 3, 4-tetrahydroisoquinoline to 3, 4-dihydroisoquinolines. The results show that ZnIn2S4 synthesized in ethylene glycol solvent has the best photocatalytic dehydrogenation activity. [ABSTRACT FROM AUTHOR]