The reaction between the ((E)-N′-(2-hydroxy-3-methoxybenzylidene)pyrazine-2-carbohydrazide) (H2opch) ligand and the metallo-precursor [Dy(hfac)3]·2H2O led to the formation of an homometallic coordination complex with the formula [Dy2(hfac)3(H2O)(Hopch)2][Dy(hfac)4] (1). In presence of both [Dy(hfac)3] 2H2O and the Fe(II) salt, the heterobimetallic tetranuclear [FeDy3(hfac)8(H2O)2(opch)2] (2) was isolated, while the addition of the co-ligand 1,2-Bis(2-hydroxy-3-methoxybenzylidene) hydrazine (H2bmh) led to the formation of two heterobimetallic tetranuclear complexes with the formula [Fe3Dy(hfac)6(opch)2(H2bmh)] C6H14 (3) C6H14 and [Fe2Dy2(hfac)7(opch)2(H2bmh)] 0.5C7H16 (4) 0.5C7H16. Single crystal X-ray diffraction and dc magnetic investigation demonstrated that 3 and 4 involved the iron center in the +II and +III oxidation states. Dynamic magnetic measurements highlighted the single-molecule magnet behavior of 1 and 2 in a zero applied dc field primarily due to the ferromagnetic interactions taking place in these compounds. © 2023 by the authors.