A series of novel heterostructured hybrid layered ZnO and MoS2 nanosheets composites were successfully prepared with different MoS2 contents. Among all the prepared materials, ZnO/MoS2 (1:0.05) composite showed enhanced photocatalytic activity for methylene blue degradation under direct solar light compared with pristine ZnO. The MoS2 component played a key role for the visible light activity of the composite system at longer wavelengths. The kinetic equations of photocatalytic reaction and possible photocatalytic degradation mechanism were investigated. The results indicated that it belongs to the zero order kinetic and the photogenerated electrons are transferred from hybrid layered ZnO to the MoS2 nanosheets, facilitating an interfacial electron transfer suppressing the recombination of charge carriers during the photocatalytic degradation.