Exploring effective method to optimize the photoelectronic properties of functional materials is crucial for advancing the next-generation optoelectronic devices. However, existing modulation strategies are frequently plagued by drawbacks including complex fabrication processes. However, traditional regulation approaches often suffer complex processing, and the intrinsic relationship between structural evolution and performance enhancement in one-dimensional transition-metal dichalcogenides (TMDs) under extreme conditions is still unclear, thereby hindering further performance improvement. In this study, high pressure is used as a continuously tunable and clean external field to regulate the structural and photoelectric properties of one-dimensional transition-metal dichalcogenide nanotubes (NT-WS₂). Utilizing a diamond anvil cell (DAC) combined with in situ high-pressure photocurrent measurements, Raman spectroscopy, and X-ray diffraction (XRD), we systematically investigate the pressure-dependent evolution of the crystal structure and photoelectric performance.The results show a remarkable pressure-driven enhancement in the optoelectronic response of NT-WS₂. With the increase of pressure, the device responsivity exhibits a dramatic rise from the initial 0.53 A/W to 43.75 A/W at 13.5 GPa—nearly two orders of magnitude higher. Correspondingly, the external quantum efficiency (EQE) and specific detectivity (D*) are enhanced by approximately 67-fold and 10-fold, respectively. The synergistic in situ spectroscopic and structural analyses indicate that this significant improvement arises from pressure-induced bandgap narrowing caused by strengthened interlayer interactions, along with improved carrier transport enabled by the compact stacking of nanotubes. This work not only deepens the understanding of the optoelectronic evolution mechanisms of 1D TMDs under extreme conditions but also provides a novel regulatory strategy to guide the design and optimization of high-performance nano-optoelectronic devices.