As a result of high doses of paramagnetic gadolinium (Gd) chelates administered in magnetic resonance imaging (MRI) exams, their unmetabolized excretion, and insufficient removal in wastewater treatment plants (WWTPs), large amounts of anthropogenic Gd (Gdanth) are released into surface water. The upward trend of gadolinium-based contrast agent (Gd-CA) administrations is expected to continue growing and consequently higher and higher anthropogenic Gd concentrations are annually recorded in water resources, which can pose a great threat to aquatic organisms and human beings. In addition, the feasibility of Gd retention in patients administered with Gd-CAs repeatedly, and even potentially fatal diseases, including nephrogenic systemic fibrosis (NSF), due to trace amounts of Gd have recently arisen severe health concerns. Thus, there is a need to investigate probable adverse health effects of currently marketed Gd-CAs meticulously and to modify the actual approach in using Gd contrast media in daily practice in order to minimize unknown possible health risks. Furthermore, the employment of enhanced wastewater treatment processes that are capable of removing the stable contrast agents, and the evaluation of the ecotoxicity of Gd chelates and human exposure to these emerging contaminants through dermal and ingestion pathways deserve more attention. On the other hand, point source releases of anthropogenic Gd into the aquatic environment presents the opportunity to assess surface water—groundwater interactions and trace the fate of wastewater plume as a proxy for the potential presence of other microcontaminants associated with treated wastewater in freshwater and marine systems.