Due to their enhanced light absorption efficiency, one-dimensional (1D) transition metal dichalcogenide (TMDC) nanoscrolls derived from two-dimensional (2D) TMDC nanosheets have shown excellent optoelectronic properties. Currently, organic solvent and alkaline droplet-assisted scrolling methods are popular for preparing TMDC nanoscrolls. Unfortunately, the adsorption of organic solvent or alkaline impurities on TMDC is inevitable during the preparation, which affects the optoelectronic properties of TMDC. In this work, we report a solvent-free method to prepare closely packed MoS 2 nanoscrolls by dragging a deionized water droplet onto the chemical vapor deposition grown monolayer MoS 2 nanosheets at 100 °C (referred to as MoS 2 NS-W). The as-prepared MoS 2 NS-W was well characterized by optical microscopy, atomic force microscopy, and ultralow frequency (ULF) Raman spectroscopy. After high temperature annealing, the height of MoS 2 nanoscrolls prepared using an ethanol droplet (referred to as MoS 2 NS-E) greatly decreased, indicating the loss of encapsulated ethanol in MoS 2 NS-E. While the height of MoS 2 NS-W was almost unchanged under the same conditions, implying that no water was embedded in the scroll. Compared to the MoS 2 NS-E, the MoS 2 NS-W shows more ULF breathing mode peaks, confirming the stronger interlayer interaction. In addition, the MoS 2 NS-W shows a higher Young's modulus than MoS 2 NS-E, which could arise from the closely packed scroll structure. Importantly, the MoS 2 NS-W device showed a photosensitivity 1 order of magnitude higher than that of the MoS 2 NS-E device under blue, green, and red lasers, respectively. The decreased photosensitivity of MoS 2 NS-E was attributed to the larger dark current, which might be assigned to the adsorbed ethanol between the adjacent layers in MoS 2 NS-E. Our work provides a solvent-free method to prepare closely packed MoS 2 nanoscrolls at large scale and demonstrates their great potential for high-performance optoelectronic devices.