Abstract: Infrared spectra of nontronite reveal shifts to lower wave, number in peaks located at 3570, 1030, and 821 cm−1, which are assigned to vibrational modes for O-H stretching, Si-Ob (basal oxygens) tetrahedral vibrations, and FeO-H deformation, respectively, as the Fe2+ content increases upon reduction. A pleochroic shoulder at 1110 cm−1 resulting from Si-Oa (apical oxygens) interactions appears to be unchanged with reduction. The absorption band at 848 cm−1 shifts to higher energy with reduction of structural iron, and persists at 840 cm−1 after complete deuteration of structural hydroxyls. The band is assigned to a Fe-OH mode where the OH moves as a unit. The shift in the Si-Ob mode to lower vibrational energy with reduction may indicate a decrease in stress forces between the tetrahedral and octahedral sheets.