Topological semimetals have attracted flourishing interest as promising candidates for their unique advantages in achieving highly sensitive, low-energy photodetection with ultrafast operation. Although various semimetals have been explored recently, new semimetals are still being pursued for high-responsivity photodetectors with broadband response. Here, a pressure-induced semiconductor-semimetal transition is observed in two-dimensional wide-band semiconducting lead iodide (PbI 2 ). The photocurrent under visible light shows abrupt increases by two orders of magnitude at ≈25 GPa, where the crystalline structure transforms from the Pnma to I4/MMM phase. Meanwhile, the responding band expands from visible light to at least the telecom wavelength 1550 nm. The high-pressure absorption spectra of PbI 2 suggest that the electrical band is closed at the transition point, while the charge transport shows that the sample is still not metallic. Through first-principles calculations, the photocurrent spurt and infrared band response are attributed to the appearance of a semimetal phase at high pressure, which well explains the nonmetallic transport. The prominent drop in lifetime to a few picoseconds in ultrafast spectroscopy under pressure further confirms the semiconductor-semimetal transition in PbI 2 . Pressure-induced semimetallization opens a new strategy for designing a high-performance photodetector with broadband response.