Uranium sulfide belongs to a class of uranium monochalcogenides that crystallize in the rocksalt structure and exhibit ferromagnetism at low temperature. The magnetism is believed to play a role in the low-temperature rhombohedral distortion, possibly due to its large magnetic anisotropy. We have performed electrical and structural characterization along with density-functional theory calculations as functions of pressure to help understand the interplay between structure and magnetism in US. Theoretical calculations suggest that ferromagnetic order is responsible for the small distortion at ambient pressure and low temperature. Under pressure, the Curie temperature is reduced monotonically until it discontinuously disappears near a pressure-induced deformation of the crystal structure. This high-pressure distortion is identical to the one correlated with the onset of magnetic order, but with a larger change in the cell angle. Calculations imply a reduction in the electronic band energy as the driving force for the pressure-induced structure, but the loss of magnetic order associated with this distortion remains a mystery. The high-pressure electronic phase diagram may shed light on the magnetostructural free energy landscape of US. © 2013 American Physical Society.