Reported here is a water-soluble ligand, N-(sulfoethyl)-iminodiacetic acid (H3SEIDA), used for the complexation of uranyl ions. A coordination compound composed of uranyl cation and N-(sulfonatoethyl)-ammoniodiacetate (SEADA2−) zwitterion was synthesized from an acidic aqueous solution. This compound features a 2D undulating fes (4.82) coordination layer that is stacked and linked by hydrogen-bonding interaction to form a 3D supramolecular framework with a 1D larger-cycle channel. Thermal analysis demonstrates the relatively weak bonding between uranyl cation and SEADA2− zwitterion. The monomeric uranyl-based fluorescence emission is red-shifted by about 5 nm compared to that of uranyl nitrate hexahydrate. The hydrothermal synthesis of this uranyl compound was successfully applied to the sequestration of uranyl ions.