Two　new　heterometallic　uranyl-organic　frameworks　(UOFs),　[Cd(phen)(2)(H2O)(2)][(UO2)(2)(BDC)(3)]center　dot　2H(2)O　(1)　and　[Ni(phen)(3)][(UO2)(2)(BDC)(3)]center　dot　2H(2)O　(2),　were　obtained　under　hydrothermal　conditions.　Both　crystal　structures　were　characterized　by　single-crystal　X-ray　diffraction　analyses　and　the　results　indicate　that　both　complexes　feature　a　similar　2D　honeycomb　framework　that　is　connected　by　rigid　benzenedicarboxylate　(BDC)　ligands　and　uranyl　units.　BDC　works　as　a　linker　to　bridge　neighboring　UO22+　units,　where　UO22+　is　tris-chelated.　Different　guest　molecules　guided　the　stacking　of　2D　layers　and　lead　into　their　3D　supramolecular　crystal　structures　with　different　space　groups.　As　a　result,　1　crystallized　in　a　polar　space　group　Cc,　whereas　2　belongs　to　a　chiral　space　group　P6(1)22.　Thermogravimetric　measurements　were　performed　to　study　their　thermal　stability.　UV-visible　diffuse　reflectance　spectroscopy　measurements　indicate　an　experimental　optical　bandgap　of　3.87　eV　and　3.63　eV,　respectively,　for　1　and　2.　Luminescent　studies　of　both　samples　show　strong　green　light　emissions.