The use of pelitic geological materials for the treatment of muscle-bone-skin pathologies, by application of a cataplasm made of clay and mineral water mixture, is currently receiving attention and interest from the general public and scientific community. In Portugal there are several natural occurrences of clays/muds which are used for pelotherapy and/or geotherapy. These are carried out either indoors (thalassotherapy and thermal centres) or outdoors, in natural sites generally located near the seaside. The aim of this study is to assess the mineralogical and physicochemical properties of Portuguese raw materials for therapeutic purposes. These materials were collected from different Portuguese Mesozoic-Cenozoic geological formations located in the neighbourhood of thermal centres or at beaches known from their empirical applications. X-ray diffraction (XRD) and scanning electron microscopy (SEM-EDS) were used to assess the mineralogical composition of these clays. Physicochemical properties, such as specific surface area, cation exchange capacity, plasticity/abrasiveness indices and heat diffusiveness were also determined. Having distinct geological ages and genesis, the materials examined are mainly illitic. Less abundant kaolinite and smectite are also present. With respect to their physicochemical properties, all samples have good thermal properties which make them potentially suitable for therapeutic or aesthetic purposes.