Abstract: Mössbauer and i.r. spectra of a series of nontronites show that Fe³⁺ and Al³⁺ are distributed between tetrahedral and octahedral sites. The Mössbauer results have reaffirmed the occupation by Fe³⁺ of octahedral sites at which these ions are coordinated to pairs of OH groups in both cis and trans configurations. The distribution of Fe³⁺ between these two sites varies considerably but in all of the nontronites some Fe³⁺ occurs in the trans site in contrast to the all cis occupancy of the centro-symmetric structure proposed by Mering and Oberlin (1967). In one of the nontronites the distribution of Fe³⁺ between these two sites approaches that in the ideal non-centrosymmetric structure proposed for montmorillonite.