Molybdenum disulfide (MoS2) has recently gained attention due to the exciting and various nanostructures created by different synthesis processes and their superior physical and chemical properties. Although large‐scale production with various nanostructures is achieved, only patterned film growth is demonstrated in specific locations. Traditional photolithography and etching processes are not suitable for patterning of 3D structures due to the huge height difference. The large‐scale patterned growth of MoS2 with different nanostructures is critical for sophisticated, customized electronic and optoelectronic devices. Herein, for the first time, the synthesis of large‐scale and patterned MoS2 nanosheets with vertically standing morphology (v‐MoS2 NS) using a chemical vapor deposition (CVD) method and a TiO2‐induced layer is reported. This method enables the preparation of patterned v‐MoS2 NS arrays with clean boundaries, uniform distributions, controllable locations, and various shapes, which can be used to fabricate various functional devices without etching. Next, it is demonstrated that the photodetectors can be fabricated directly using square‐patterned v‐MoS2 NS arrays. The method proposed could be extended to form other 2D materials with vertical NS structures and provides a lot of new chances to legitimately design functional devices and systems in the future.