A series of isostructural three-dimensional metal-organic frameworks [Pr(2)(N-BDC)(3)(dmf)(4)](infinity) (1), {[Eu(2)(N-BDC)(3)(dmf)(4)] x 2DMF}(infinity) (2 x 2DMF), [Gd(2)(N-BDC)(3)(dmf)(4)](infinity) (3), {[Tb(2)(N-BDC)(3)(dmf)(4)] x 2DMF}(infinity) (4 x 2DMF), {[Dy(2)(N-BDC)(3)(dmf)(4)] x 2DMF}(infinity) (5 x 2DMF) (N-H(2)BDC = 2-amino-1,4-benzenedicarboxylic acid; DMF = N,N'-dimethylformamide) with cubic 4(12) x 6(3) topology have been synthesized using solvothermal conditions. The networks were generated via formation of a dinuclear Ln(2) secondary building block, involving the dicarboxylate ligand as a bridge. The luminescent properties of the Tb(III) and Eu(III) complexes were studied and showed characteristic emissions at room temperature. Antiferromagnetic interactions between Ln(III) ions were observed from magnetic susceptibility data.