A novel uranyl-organic framework [(CH3)(2)NH2][UO2(TATAB)]center dot 2DMF center dot 4H(2)O (U-TATAB) was assembled through the solvothermal synthesis of UO2(CH3COO)(2)center dot 2H(2)O and triazine tricarboxylate linker H(3)TATAB (H(3)TATAB = 4,4',4 ''-s-triazine-1,3,5-triyltri-p-aminobenzoate). It was characterized by single-crystal X-ray diffraction, elemental analysis, IR, powder X-ray diffraction, and thermogravimetric microanalysis. It is worth mentioning that U-TATAB exhibits an original arrangement of structures with interesting topology. Structural analysis confirmed that U-TATAB displays an interesting two-dimensional graphene-like layered topology. In order to broaden its functional characteristics, we first investigated the functional adsorbent U-TATAB for iodine capture in cyclohexane solution and for the removal of dye in aqueous solution. Large porosity, unique structure character, and the pi-electron walls made of TATAB make the material a promising functional absorbent exhibiting excellent adsorption performance for iodine and dye molecules. Most notably, this is the first case of a uranyl-organic framework built by secondary building unit (SBU) [UO2(RCOO)(3)](-) and extended trigonal triazine tricarboxylate ligand H(3)TATAB with amino functional groups.