Nanostructures of layered 2D materials have been proven one of the significant recent trends for visible-light-driven photocatalysis because of their unique morphology, effective optical adsorption, and rich active sites. Herein, we synthesized ultrathin-layered MoS2 nanoflowers and nanosheets with rich active sites by using a facile hydrothermal technique. The photocatalytic performance of the as-synthesized MoS2 nanoflowers (NF) and nanosheets (NS) were investigated for the photodegradation of MB (methylene blue), MG (malachite Green), and RhB (rhodamine B) dye under visible light irradiations. Ultrathin-layered nanoflowers showed faster degradation (96% in 150 min) in RhB under visible light irradiation, probably due to a large number of active sites and high available surface area. The kinetic study demonstrated that the first-order kinetic model best explained the process of photodegradation. The MoS2 nanoflowers catalysts has similar catalytic performance after four consecutive cyclic performances, demonstrating their good stability. The results showed that the MoS2 nanoflowers have outstanding visible-light-driven photocatalytic activity and could be an effective catalyst for industrial wastewater treatment. © 2022 American Chemical Society. All rights reserved.