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Supported nanostructured photocatalysis is considered to be a sustainable and promising method for water pollution photodegradation applications due to its fascinating features, including a high surface area, stability against aggregation, and easy handling and recovery. However, the preparation and morphological control of the supported nanostructured photocatalyst remains a challenge. Herein, a one-step hydrothermal method is proposed to fabricate the supported vertically aligned ZnO nanosheet arrays based on aluminum foil. The morphologically controlled growth of the supported ZnO nanosheet arrays on a large scale was achieved, and the effects of hydrothermal temperature on morphologic, structural, optical, and photocatalytic properties were observed. The results reveal that the surface area and thickness of the nanosheet increase simultaneously with the increase in the hydrothermal temperature. The increase in the surface area enhances the photocatalytic activity by providing more active sites, while the increase in the thickness reduces the charge transfer and thus decreases the photocatalytic activity. The influence competition between the area increasing and thickness increasing of the ZnO nanosheet results in the nonlinear dependence between photocatalytic activity and hydrothermal temperature. By optimizing the hydrothermal growth temperature, as fabricated and supported ZnO nanosheet arrays grown at 110 °C have struck a balance between the increase in surface area and thickness, it exhibits efficient photodegradation, facile fabrication, high recyclability, and improved durability. The RhB photodegradation efficiency of optimized and grown ZnO nanosheet arrays increased by more than four times that of the unoptimized structure. With 10 cm 2 of as-fabricated ZnO nanosheet arrays, the degradation ratio of 10 mg/L MO, MB, OFL, and NOR was 85%, 51%, 58%, and 71% under UV irradiation (365 nm, 20 mW/cm 2 ) for 60 min. All the target pollutant solutions were almost completely degraded under UV irradiation for 180 min. This work offers a facile way for the fabrication and morphological control of the supported nanostructured photocatalyst with excellent photodegradation properties and has significant implications in the practical application of the supported nanostructured photocatalyst for water pollution photodegradation.