The clay mineralogy and chemistry of a green lacustrine marl that has been pedogenically modified in the upper part was investigated in order to better understand the formation of low-temperature Fe-rich 10 Å clay. Twelve samples in a vertical sequence have been investigated using X-ray diffraction (XRD), chemical analysis, scanning electron microscopy (SEM) and laser particle size analysis. The clay assemblage has a range of overall illite-smectite (I-S) compositions (64–100%) resulting from several I-S phases that, for the sake of modelling, have been simplified to one to three I-S phases of increasing illitic content. Where the lacustrine marl has been pedogenically modified, the smectite-rich I-S is much reduced in abundance or absent and the 10 Å -rich component is both more abundant and more illitic. These assemblages are a consequence of illitization of detrital I-S in the lake and soil, and dissolution of other clays (kaolinite and chlorite) in the hypersaline lake. Interlayer K, octahedral Fe and octahedral + interlayer Mg increase with intensity of illitization (increase range 0.32–0.63, 0.68–1.67, 0.18–0.24 per O10(OH)2, respectively), first in the increasingly saline lake, and latterly as a result of wetting and drying in a gley soil. In the soil environment, reduction of Fe(III) to Fe(II) resulted in increased layer charge but, as by this stage very few smectite interlayers remained, this did not result in an equivalent increase in illite. Laser particle-size analysis, supported by SEM observation, shows the existence of a bimodal distribution of clay particle size (maxima at 0.2 and 1.5–1.8 μm) in which the finer fraction increases largely in the pedogenically affected samples, probably due to particle break-up caused by seasonal wetting and drying. This ‘dual action’ illitization, first in a hypersaline lake and latterly through wetting and drying, may be responsible for both the intensity of illitization and exceptionally high (for the Solent Group) Fe content of the authigenic illite. The chemical characteristics of the illitic I-S and the illite end-member correspond to glauconite. Hence, this is an example of onshore, non-pelletal glauconite formation.