The mineral amarantite Fe2(3+)(SO4)O·7H2O has been studied using a combination of techniques including thermogravimetry, electron probe analyses and vibrational spectroscopy. Thermal analysis shows decomposition steps at 77.63, 192.2, 550 and 641.4°C. The Raman spectrum of amarantite is dominated by an intense band at 1017 cm(-1) assigned to the SO4(2-) ν1 symmetric stretching mode. Raman bands at 1039, 1054, 1098, 1131, 1195 and 1233 cm(-1) are attributed to the SO4(2-) ν3 antisymmetric stretching modes. Very intense Raman band is observed at 409 cm(-1) with shoulder bands at 399, 451 and 491 cm(-1) are assigned to the ν2 bending modes. A series of low intensity Raman bands are found at 543, 602, 622 and 650 cm(-1) are assigned to the ν4 bending modes. A very sharp Raman band at 3529 cm(-1) is assigned to the stretching vibration of OH units. A series of Raman bands observed at 3025, 3089, 3227, 3340, 3401 and 3480 cm(-1) are assigned to water bands. Vibrational spectroscopy enables aspects of the molecular structure of the mineral amarantite to be ascertained.