A single-crystal sample of galenobismutite was subjected to hydrostatic pressures in the range of 0.0001 and 9 GPa at room temperature using the diamond-anvil cell technique. A series of X-ray diVraction intensities were collected at ten distinct pressures using a CCD equipped 4-circle diVractometer. The crystal structure was reWned to R1(|F₀| > 4s) values of approximately 0.05 at all pressures. By Wtting a third-order Birch-Murnaghan equation of state to the unit-cell volumes V₀ = 700.6(2) ų, K₀ = 43.9(7) GPa and dK/dP = 6.9(3) could be determined for the lattice compression. Both types of cations in galenobismutite have stereochemically active lone electron pairs, which distort the cation polyhedra at room pressure. The cation eccentricities decrease at higher pressure but are still pronounced at 9 GPa. Galenobismutite is isotypic with CaFe₂O₄ (CF) but moves away from the idealised CF-type structure during compression. Instead of the two octahedral cation sites and one bi-capped trigonal-prismatic site, PbBi₂S₄ attains a new high-pressure structure characterised by one octahedral site and two mono-capped trigonal-prismatic sites. Analyses of the crystal structure at high pressure conWrm the preference of Bi for the octahedral site and the smaller one of the two trigonal-prismatic sites.