Abstract The transition metal chalcogenide Cr2S3-x has unique properties, such as a lower antiferromagnetic transition temperature, semiconducting behavior, and thermoelectric properties. We focus on the effects of high pressure on the properties of electrical transport and structure in the single crystal Cr2S2.88. It is observed that the resistance drops abruptly by approximately two orders of magnitude and the temperature derivative of the resistance changes from negative to positive after 15.7 GPa. The Cr2S2.88 crystal has undergone transitions from a semiconductor-like phase to a metal I phase and then to another metal II phase. Simultaneously, a structural phase transition after 16.1 GPa is confirmed by synchrotron angle dispersive X-ray diffraction (AD-XRD). After the structural phase transition, the negative magnetoresistance becomes positive with increasing pressure and shows a linear relationship in the metal II phase. Electron-type carriers dominate in the semiconductor-like phase, but hole-type carriers dominate after the structural phase transition. Our work provides an example of the effective modulation of semiconductor-like properties by pressure, which is meaningful for the innovation and development of semiconductor technology.