The growing awareness of energy conservation has stimulated intensive research activities toward solar energy utilization. It is predicted that the annual average CO 2 concentration for 2021 is 416.3 ppm (AE0.6), which is the first year on record that sees CO 2 levels of more than 50% above preindustrial levels, indicating the urgency of the global environmental burdens. [1] Since the pioneering utilizing n-type TiO 2 electrode to produce H 2 via photoelectrochemical water splitting by Fujishima and Honda in 1972, semiconductor photocatalysis technology is considered as one of the fascinating technologies to alleviate energy problems. [2] With the development of research in recent years, photocatalytic reduction reaction (such as photocatalytic water splitting, CO 2 reduction, and nitrogen fixation) has been paid more and more attention to solve the critical issues related to energy and the environment. However, photocatalyst with large bandgap energy, such as TiO 2 , remains the bottleneck to satisfy the practical application owing to the low efficiency of solar energy utilization. [3,4] Therefore, extensive efforts have been undertaken to develop visible-lightirradiated photocatalysts that can better utilize solar energy. Until now, various visible-light photocatalysts have been invented by the researchers, such as simple oxides (Fe 2 O 3 ), [5] graphitic carbon nitride (g-C 3 N 4 ), [6][7][8][9] complex oxides (Bi 2 WO 6 ), [10] and metal chalcogenides (CdS). [11] In recent years, metal chalcogenides have been extensively investigated as the next-generation photocatalyst for their excellent optoelectronic and catalytic properties. [12] Zinc indium sulfide (ZnIn 2 S 4 ), a novel ternary metal chalcogenide, has been applied in many applications due to its outstanding properties (Figure 1). It is a layered structure photocatalyst with three major