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In the title heteronuclear ZnII—TbIII complex (systematic name: {6,6′-dimethoxy-2,2′-[ethane-1,2-diylbis(nitrilomethylidyne)]diphenolato-1κ4O6,O1,O1′,O6′}:2κ4O1,N,N′,O1′-μ-nitrato-1:2κ2O:O′-dinitrato-1κ4O,O′-terbium(III)zinc(II)), [TbZn(C18H18N2O4)(NO3)3], with the hexadentate Schiff base compartmental ligand N,N′-bis(3-methoxysalicylidene)ethylenediamine (H2L), the Tb and Zn atoms are triply bridged by two phenolate O atoms of the Schiff base ligand and one nitrate ion. The five-coordinate Zn atom is in a square-pyramidal geometry with the donor centers of two imine N atoms, two phenolate O atoms and one of the bridging nitrate O atoms. The TbIII center has a ninefold coordination environment of O atoms, involving the phenolate O atoms, two methoxy O atoms, two O atoms from two nitrate ions and one from the bridging nitrate ion. Weak intermolecular C—H...O interactions generate a two-dimensional layer structure.