209Bi-aryl compounds have the potential for designing novel class of smart MRI T1 contrast agents which are sensitive to the chemical environment and the B0 field. We have confirmed quadrupolar relaxation enhancement (QRE) of protons as the underlying mechanism in two solid organobismuth-compounds in the B0 range 0.5 – 3T. We also show first QRE peaks of solvent protons in a solution of Tris-(2-orthomethoxy-Phenyl)Bismuthane in tetrahydrofurane. This very important first step yields two promising candidates for the development of QRE-based CAs and opens the way for the second step, i.e. grafting them onto water-soluble nanoparticles for optimizing the relaxivity.