The molecular structure of the uranyl mineral rutherfordine has been investigated by the measurement of its Raman spectra at 298 and 77 K and complemented with infrared spectra. The infrared spectra of the (CO3)(2-) units in the anti-symmetric stretching region show complexity with three sets of carbonate bands observed. This, combined with the observation of multiple bands in the (CO3)(2-) bending region in both Raman and IR spectra, suggests that both monodentate and bidentate (CO3)(2-) units are present in the structure in accordance with the X-ray crystallographic studies. Complexity is also observed in the IR spectra of (UO2)(2+) anti-symmetric stretching region and is attributed to non-identical UO bonds. Both Raman and infrared spectra of the rutherfordine show the presence of both water and hydroxyl units in the structure, as evidenced by IR bands at 3562 and 3465 cm(-1) (OH) and 3343, 3185 and 2980 cm(-1) (H2O). Raman spectra show the presence of four sharp bands at 3511, 3460, 3329 and 3151 cm-1. Copyright (C) 2007 John Wiley & Sons, Ltd.