As an emergent van der Waals multiferroic semiconductor of CuCrP2⁢S6 (CCPS), its high-temperature and high-pressure structural, ferroelectric, and electrical transport properties were comprehensively studied at 298–873 K and 0.8–45.0 GPa using an externally heated diamond-anvil cell joined with Raman spectroscopy, electrical conductivity, and high-resolution transmission electron microscopy observations under different hydrostatic environments. For nonhydrostatic compression of CuCrP2⁢S6, two sequential structural transitions at 5.6 and 13.6 GPa took place, followed by a semiconductor-to-metal crossover at 28.6 GPa. Nevertheless, the pressure-driven structural transition and metallization of CuCrP2⁢S6 were delayed by ∼2.0GPa under hydrostatic condition owing to the influence of defects and dislocation. Upon depressurization, the phase transformation of CCPS was demonstrated to be reversible under different hydrostatic environments. Additionally, the linearity between electrical current and sinusoidal voltage with the nonlinearity factors of ∼1.00 manifested the Ohmic response of CuCrP2⁢S6 under high pressure. Simultaneously, the noticeable discontinuities in temperature-dependent Raman shifts, full width at half maximums Raman peak intensity ratios, and electrical conductivity at 423 K provided robust evidence of the ferroelectric transition of CCPS at ∼0.4 GPa. These findings on CuCrP2⁢S6 offer insight into the interplay of crystalline structure, electric polarization, and electrical transport behavior for two-dimensional multiferroic materials under high-temperature and high-pressure conditions and stimulate the potential development of advanced multifunctional devices.