The crystal and magnetic structures of van der Waals layered antiferromagnet $\mathrm{Cr}{\mathrm{Cl}}_3$ have been studied using x-ray and neutron powder diffraction at pressures up to 15 GPa at ambient temperature and up to 2 GPa in a temperature range 7–300 K, respectively. The vibrational properties of $\mathrm{Cr}{\mathrm{Cl}}_3$ were studied using Raman spectroscopy at pressures up to 28 GPa at ambient temperature. Application of high pressure leads to a gradual structural phase transition from the monoclinic $C2$/m to rhombohedral $R\overline{3}$ structure developed in the pressure range of 1–6 GPa at ambient temperature. It is accompanied by anomalies in the pressure behavior of lattice parameters, unit cell volume, and vibrational modes. Upon compression above 1 GPa at low temperatures, the initial A-type antiferromagnetic state becomes suppressed, and the ferromagnetic state is formed below Curie temperature $T_{\mathrm{C}}\sim 19$ K. The microscopic nature of the pressure-induced AFM–FM magnetic phase transition in bulk $\mathrm{Cr}{\mathrm{Cl}}_3$ is different from those found in bilayer $\mathrm{Cr}{\mathrm{I}}_3$. These findings clarify, in detail, a response of structural and magnetic states in a model $\mathrm{Cr}{\mathrm{Cl}}_3$ system with the AFM ground state on variation of thermodynamic parameters and provide important information for further development of theoretical models describing physical properties of chromium trihalides and related van der Waals materials in bulk and few-layered forms.

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• Magnetic order
• Phase transitions
• Pressure effects
• Structural properties
• Layered crystals
• Neutron diffraction
• Raman spectroscopy
• X-ray diffraction