Metal tetraphosphides (MP 4 , M ¼ 3d transition metals) exhibit the layeredstructure character, in which the metal atom chains are sandwiched between the P 4 2À layers, and have attracted considerable interest due to the outstanding physical and chemical properties, such as good electrical conductivity and high lithium capacity. Herein, the CrP 4 single crystal is prepared using the highpressure and high-temperature method via the 2000 ton Kawai-type multianvil apparatus at ShanghaiTech University (SHTech-2000). The structural modification under high pressure is investigated by synchrotron X-ray diffraction combined with diamond anvil cell techniques. CrP 4 shows remarkable axial anisotropic compressibility, in which the c-axis is more compressible than aand b-axes. The formation of infinite chains of Cr─Cr metallic bonding in CrP 4 under high pressure enhances the electrical conductivity.