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Some landslides around the world that have low-angle failure planes show exceptionally poor mechanical properties. In some cases, an extraordinarily pure clay layer has been detected on the rupture surface. In this work, a complex landslide, the so-called Diezma landslide, is investigated in a low- to moderate-relief region of Southeast Spain. In this landslide, movement was concentrated on several surfaces that developed on a centimeter-thick layer of smectite (montmorillonite-beidellite) clay-rich level. Since these clayey levels have a very low permeability, high plasticity, and low friction angle, they control the stability of the entire slide mass. Specifically, the triggering factor of this landslide seems to be linked to the infiltration of water from a karstic aquifer located in the head area. The circulation of water through old failure planes could have promoted the active hydrolysis of marly soils to produce new smectite clay minerals. Here, by using geophysical, mineralogical, and geochemical modelling methods, we reveal that the formation and dissolution of carbonates, sulfates, and clay minerals in the Diezma landslide could explain the elevated concentrations of highly plastic secondary clays in its slip surface. This study may help in the understanding of landslides that show secondary clay layers coinciding to their low-angle failure planes.