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Here, we report significant pressure-modulate optoelectronic properties of NiPS3. Upon compression, NiPS3 exhibited a photocurrent increase of five orders of magnitude over the initial value. Interestingly, when NiPS3 was finally decompressed to ambient conditions, the photocurrent could maintain a two-order-of-magnitude enhancement. In addition, the spectral response range was extended to the near-infrared spectral range (up to 1650 nm) under high pressure. Raman and XRD measurements and theoretical calculations revealed significant enhancement in both interlayer and intralayer interactions during compression, leading to a remarkable modulation of the optoelectronic properties. By applying pressure, giant enhancement of photocurrent and tunable spectral response range were achieved in NiPS3, which provides a potential way to modify the optoelectronic properties for materials. [ABSTRACT FROM AUTHOR]