A tripodal ligand based on the 8-hydroxyquinolinate binding unit yields a soluble and highly stable bis-hydrated Gd3+ complex in water (pGd = 19.2(3)) with relaxivity change in the pH range 4.5-7.4 and Nd3+, Yb3+ analogues with sizeable NIR emission upon excitation at 370 nm providing a new architecture for the development of bimodal agents. © 2010 The Royal Society of Chemistry.