Hypothesis: The objective is to elucidate the multiscale dynamics of water within natural mixtures of minerals, green earth pigments that are mainly composed of phyllosilicates containing large amount of iron. In particular, the interaction of water with the different kinds of surfaces has to be probed. One issue is to examine the influence of surface type, basal or edge, on the dispersion quality. Experiment: The study was carried out using 1H variable field NMR relaxometry on various green earth pigment dispersions and concentrations. To analyse the data, a new analytical model was developed for natural phyllosilicates containing large amount of paramagnetic centres. Finding: The proposed theoretical framework is able to fit the experimental data for various samples using few parameters. It allows to determining water diffusion and residence times in complex phyllosilicate dispersions. Furthermore, it makes it possible to differentiate the contribution of the basal and edge surfaces and their respective surface area in interaction with water. Moreover, NMR relaxation profile reveals to be highly sensitive to the structural aspect of the phyllosilicates and to the accessibility of water to iron, hence allowing to discriminate clearly between two very similar phyllosilicates (glauconite and celadonite) that are difficult to distinguish by standard structural methods.