Nanoscale transition-metal dichalcogenide materials showed promising potential for visible-light responsive photocatalysis. Here, we report our investigations on the synthesis of heterodimensional nanostructures of two-dimensional (2D) ultrathin MoS nanosheets interspersed with ZnO nanoparticles by using a facile two-step method consisting of sonication-aided exfoliation technique followed by a wet chemical process. The photocatalytic activity of the nanocomposites was examined by studying the degradation of different organic dye pollutants and tetracycline, a common antibiotic, under visible-light irradiation. It is found that within 30 min more than 90 % of the model organic dye was photodegraded by the optimized quasi-0D/2D hybrid nanomaterial. The reaction rate of pollutant degradation is about five and eight times higher than those of the pristine MoS naonosheets and P25 photocatalysts, respectively. The outstanding photocatalytic activity of the heterodimensional hybrids can be attributed to a few beneficial features from the synergetic effects. Most importantly, the intimate junction between ZnO and MoS facilitates the separation of photogenerated carriers, leading to the enhancement of photocatalytic efficiency. A tentative photocatalytic degradation mechanism was proposed and tested. Overall, the present work provides valuable insights for the exploration of cost-effective nanoscale heterodimensional hybrids constructed from atomically thin layered materials.