Gadolinium-based contrast agents (GBCAs) have revolutionized medical imaging, enhancing the accuracy and diagnostic value of magnetic resonance imaging (MRI). The increasing use of GBCAs has raised concerns about the release of gadolinium (Gd)(III) into the environment and potential risks for human health. Initially, multiple administrations of GBCAs were associated only with nephrogenic system fibrosis disease in individuals with impaired kidney function. Even if the Gd(III) retention in tissues has not yet been correlated with any specific disease, caution is required for the extensive use of GBCAs. The concerns related to the employment of GBCAs, due to the possible deposition and retention, should be extended also to healthy individuals without renal impairments. To ensure the well-being of patients, there is a need to develop even more stable and better-performing GBCAs, new MRI approaches requiring lower doses of GBCAs and, finally, innovative methods for recovering Gd(III) from both patients' urines and the environment. This can have strong advantages for human health and for environmental sustainability, also considering Gd(III) scarcity, being a rare earth element, and the shared guideline to reduce, as much as possible, the use of rare metals.