An optimized microwave-assisted synthesis has been used to prepare an isotypical series of 3D Ln 3+ metal-organic frameworks (MOFs) based on residues of 2,5-pyridinedicarboxylic (pydc), namely, [Ln 2 (pydc) 3+ (1-LaEuTb). The materials can be readily isolated as microcrystals after 1 min of reaction time at 120°C. The compounds have been extensively studied in the solid state by vibrational spectroscopy (FTIR and FT-Raman), thermogravimetry, powder X-ray diffraction, elemental analysis, and electron microscopy (SEM, SEM mapping, and TEM). The structural relationships between the isolated materials and other solids reported in the literature have been investigated in detail from a structural and topological perspective with attention focused on the different connectivities of the employed organic ligand. The 3D densely packed