In the title heteronuclear Zn(II)-Sm(III) complex, [SmZn(C(18)H(18)N(2)O(4))(NO(3))(3)(CH(3)CH(2)OH)], with the hexa-dentate Schiff base compartmental ligand N,N'-bis-(3-methoxy-salicyl-idene)ethyl-enediamine (H(2)L), the Sm(III) and Zn(II) ions are triply bridged by two phenolate O atoms from the Schiff base ligand and one nitrate anion. The five-coordinate Zn(II) ion is in a square-pyramidal geometry formed by the donor centers of two imine N atoms, two phenolate O atoms and one of the bridging nitrate O atoms. The Sm(III) center is in a ten-fold coordination of O atoms, involving the phenolate O atoms, two meth-oxy O atoms, one ethanol O atom, and two O atoms from two nitrate anions and one from the bridging nitrate anion. In the crystal, inter-molecular O-H⋯O and C-H⋯O inter-actions generate a layer structure extending parallel to (101).