Raman spectroscopy of the mineral uranopilite at 298 and 77K has been obtained and used to elucidate the structure of the mineral at the molecular level. A single intense band at 1010cm −1 is assigned to the ν 1 (SO 4 ) 2− symmetric stretching mode. Three low intensity bands in the 298K Raman spectrum are observed at 1143, 1117 and 1097cm −1 and in the 77K spectrum four bands at 1148, 1130, 1118 and 1106cm −1 . These bands are attributed to the ν 3 antisymmetric stretching modes. A series of infrared bands are found at 1559, 1540, 1526 and 1511cm −1 attributed to δ UOH bending modes. Three bands are observed at 843, 835 and 819cm −1 in both 298 and 77K spectra attributed to the ν 1 symmetric stretching modes of the (UO 2 ) 2+ units. In the infrared spectra bands are observed at 941, 929 and 910cm −1 and are assigned to the ν 3 antisymmetric stretching modes of the UO 2 units. These values are used to calculate UO bond distances. Multiple OH stretching modes prove a complex arrangement of OH groupings, i.e. water molecules and OH − ions, and hydrogen bonding in the crystal structure of uranopilite.