The self-assembly of dysprosium(III) with the tailored chemical modification of the vanillin group affords two decorated Dy(3) compounds, namely, [Dy(3)(μ(3)-OH)(2)(Hpovh(-))(3)(NO(3))(3)(CH(3)OH)(2)H(2)O]·NO(3)·3CH(3)OH·2H(2)O (2) and [Dy(3)(μ(3)-OH)(2)(H(2)vovh(-))(3)Cl(2)(CH(3)OH)(H(2)O)(3)][Dy(3)(μ(3)-OH)(2)(H(2)vovh(-))(3)Cl(2)(H(2)O)(4)]·Cl(4)·2CH(3)OH·2CH(3)CN·7H(2)O (3), where H(2)povh = N-(pyridylmethylene)-o-vanilloylhydrazone and H(3)vovh = N-vanillidene-o-vanilloylhydrazone. Of particular interest is that those two title Dy(3) compounds maintain the peculiar vortex-spin structure of the ground nonmagnetic doublet. Complex 2 displays frequency-dependent slow magnetic relaxation, while 3 still inherits the single-molecule-magnet behavior as the parent Dy(3) prototype. The dissimilar dynamic magnetic behavior originates from the structural differences in light of the coordination environment of Dy(III) ions, which influence the local tensor of anisotropy and crystal-field splitting on each Dy site.