Reaction of uranyl dications with (2-carboxyethyl)(phenyl)-phosphinic acid (CPPA, H 2 L) under hydrothermal conditions gave two layered isomers (UO 2 ) 2 (L) 2 , namely, CPP-U1 and CPP-U2. Both of them feature edge-sharing uranyl dimers as structure-building units, which are ligated by CPP ligands in different ways, thus leading different layered arrangements. With the addition of imidazole derivatives, two three-dimensional structures UO 2 (L)(dib) 0.5 (CPP-U3) and UO 2 (L)(bbi) 0.5