The exquisite combination of heterometallic [Tb III Mn II (CO 2 ) 3 (H 2 O) 2 ] clusters with the hexacarboxylate ligand of H 6 TDP generates one water-stable 3D heterometallic Tb III /Mn IIorganic framework material {TbMn(HTDP)(H 2 O) 2 ]•5DMF• 4H 2 O} n (NUC-3; H 6 TDP = 2,4,6-tri(2′,4′-dicarboxyphenyl)pyridine), which consists of functionalized noninterspersed opening nanochannels shaped by six rows of [Tb III Mn II (CO 2 ) 3 (H 2 O) 2 ] clusters. Based on the single-component sorption measurements, activated NUC-3 framework exhibits effective CO 2 /CH 4 separation associated with high uptake and moderate adsorption enthalpy of CO 2 . Dynamic breakthrough experiments reveal that NUC-3 could be competent for the separation of CO 2 /CH 4 (50:50, v:v) mixture. Moreover, the kinetic and equilibrium experiments of iodine adsorption indicate that NUC-3 possess excellent adsorption capacity for iodine molecules in cyclohexane solution. The excellent structural stability and functional internal surface makes NUC-3 a prospective adsorbent for practical CO 2 /CH 4 separation and adsorption elimination of iodine molecules, opening up the insight of heterometallic MOFs for pratical application.