[Abstract] A Gd complex based on a polyphosphonated pyridyl ligand shows a very high stability in aqueous solution (logKEuL = 25.7), a high relaxivity (8.5 mM−1 s−1 at 25 °C and 20 MHz) and a marked and selective relaxivity enhancement (37%) in the presence of Mg2+, opening interesting perspectives for the design of cation responsive contrast agents