Abstract: | Two new Zn2Dy2 complexes were constructed from Zn (II) salen‐type Schiff base complex fragment and 2,6‐pyridinedimethanol (H2pdm) or its Br‐substituted analogue (4‐bromopyridine‐2,6‐diyl)dimethanol (H2Brpdm); their molecular formulas are Zn2Dy2(L)2(pdm)2(MeOH)2](ClO4)2 1 , H2L = N, N′‐ bis(3‐methoxysalicylidene)‐1,3‐diaminopropane] and Zn2Dy2(L)2(Brpdm)2(MeOH)2](ClO4)2 2 ], the Dy (III) ions of which have a NO7 triangular dodecahedral coordination sphere. The two complexes show not only ferromagnetic interaction but also field‐induced single‐molecule magnet (SMM) behavior, which are rare Dy (III)‐containing cluster complexes with the NO7 triangular dodecahedral coordination sphere that can show good magnetic relaxation. The energy barrier value of complex 2 is higher than those of complex 1 and the Dy (III) complexes with the DyNO7 triangular dodecahedral coordination configuration reported in the literature. |