Large-scale, well-aligned, and oriented ZnS nanorod arrays were fabricated by a novel and original template-free hydrothermal method. The ZnS nanorods were grown on the pulse-plating Zn nanocrystallines along a certain Zn crystalline direction. It was found that reaction factors such as hydrothermal reaction time, zinc source, and sulfide source concentration in the precursor solution, the acid–base property of the precursor solution, and the substrate where ZnS nanorod arrays were grown greatly influence the morphology of the final products. The growth mechanism of ZnS nanorod arrays was also studied. Pulse-plating Zn nanocrystallines were found to be essential for the growth of ZnS nanorod arrays. These ZnS nanorod arrays could be theoretically fabricated on almost any raw base plate as long as Zn nanocrystallines could be pulse-plated on it. Therefore, the as-synthesized ZnS nanorod array might be one of the promising candidates for field-emission or sensitive nanomaterials in the future.