The generation of two types of complexes with different topological connections and completely different structural types merely via the substitution effect is extremely rare, especially for -CH3 and -C2H5 substituents with similar physical and chemical properties. Herein, we used 3-methoxysalicylaldehyde, 1,2-cydohexanediamine, and Dy(NO3)(3)center dot 6H(2)O to react under solvothermal conditions (CH3OH:CH3CN = 1:1) at 80 degrees C to obtain the butterfly-shaped tetranuclear Dy-III cluster [Dy-4(L-1)(4)(mu(3)-O)(2)(NO3)(2)] (Dy-4, H2L1 = 6,6'-((1E,1'E)-(cyclohexane-1,3-diylbis(azanylylidene))bis(methanylylidene))bis(2-methoxyphenol)). The ligand H2L1 was obtained by the Schiff base in situ reaction of 3-methoxysalicylaldehyde and 1,2-cyclohexanediamine. In the Dy-4 structure, (L-1)(2-) has two different coordination modes: mu(2)-eta(1):eta(2):eta(1):eta(1) and mu(4)-eta(1):eta(2):eta(1):eta(2):eta(1). The four Dy-III ions are in two coordination environments: N2O6 (Dy1) and O-9 (Dy2). The magnetic testing of cluster Dy-4 without the addition of an external field revealed that it exhibited a clear frequency-dependent behavior. We changed 3-methoxysalicylaldehyde to 3ethoxysalicylaldehyde and obtained one case of a hydrogen-bonded helix framework, [DyL2(NO3)(3)](n)center dot 2CH(3)CN (Dy-HHFs, H2L2 = 6,6 1-((1E,1'E)-(cyclohexane-1,3-diylbis(azanylylidene))bis methanylylidene))bis(2-ethoxyphenol)), under the same reaction conditions. The ligand H2L2 was formed by the Schiff base in situ reaction of 3-ethoxysalicylaldehyde and 1,2-cyclohexanediamine. All Dy(III )ions in the Dy-HHFs structure are in the same coordination environment (O-9). The twisted S-shaped (L-2)(2-) ligand is linked by a Dy(III) ion to form a spiral chain. The spiral chain is one of the independent units that is interconnected to form Dy-HHFs through three strong hydrogen-bonding interactions. Magnetic studies show that Dy-HHFs exhibits single-ion-magnet behavior (U-eff = 68.59 K and tau(0) = 1.10 x 10(-7) s, 0 Oe DC field; U-eff = 131.5 K and tau(0) = 1.22 x 10(-7) s, 800 Oe DC field). Ab initio calculations were performed to interpret the dynamic magnetic performance of Dy-HHFs, and a satisfactory consistency between theory and experiment exists.