Urban aquifers are a potential alternative, with which to cover the rising demand for freshwater. However, they are commonly polluted by a wide range of anthropogenic substances, including rare earth elements (REEs). In this context, it is essential to investigate the presence and behaviour of these pollutants, in order to safely use urban groundwater. An example of these contaminants is Gadolinium, which can reach the environment after it has been used for medical purposes. Gadolinium anomalies were detected in hydraulically connected surface and subsurface water bodies in Barcelona, northeast Spain. A striking factor in this study, is that Gadolinium pollution in groundwater was less frequent and more attenuated than in surface water, suggesting that Gadolinium attenuation may be prevalent in the subsurface. Batch experiments were conducted and modelled to ascertain processes affecting Gadolinium in the sampled aquifers. Experimental results have (i) demonstrated that the concentration of dissolved Gadolinium decreased 90% in 24 days, and (ii) suggested that sorption plays a key role in Gadolinium attenuation. The modelling of the experiments provides essential parameters, with which to predict the behaviour of Gadolinium. Our results have significant implications for understanding the evolution of anthropogenic Gadolinium in aquifers in general, which is of paramount importance for determining where groundwater can be safely used after its natural or artificial infiltration.