MoSe 2 /montmorillonite composite nanosheets were successfully synthesized by a facile hydrothermal method, and the photocatalytic activities of the samples were evaluated by the decoloration of Rhodamine B. The structural characterizations indicate that the MoSe 2 nanosheets grow uniformly on the surface of montmorillonite with interface interaction, and the active sites on the nanosheet edges are exposed. Montmorillonite can inhibit the agglomeration of MoSe 2 nanosheets, improve the hydrophilicity and dispersibility of composites, and provides a larger surface area and more reactive sites for photocatalytic reaction. MoSe 2 /montmorillonite possesses the highest adsorption properties and photocatalytic abilities, and the overall decoloration rate is up to 98.2% after visible light irradiation for 45 min. The assembly of montmorillonite could enhance the photocatalytic ability of MoSe 2 , and the possible photocatalytic reaction mechanism of MoSe 2 /montmorillonite for Rhodamine B was explored. MoSe 2 /montmorillonite has potential applications in the photodegradation of organic dyes in the wastewater.