The self-assembly of dysprosium(III) with the tailored chemical modification of the vanillin group affords two decorated Dy-3 compounds, namely, [Dy-3(mu(3)-OH)(2)(Hpovh(-))(3)(NO3)(3)(CH3OH)(2)-H2O]center dot NO3 center dot 3CH(3)OH center dot 2H(2)O (2) and [Dy-3(mu(3)-OH)(2)(H(2)vovh(-))(3)Cl-2(CH3-OH)(H2O)(3)][Dy-3(mu(3)-OH)(2)(H(2)vovh-)(3)Cl-2(H2O)(4)]center dot Cl-4 center dot 2CH(3)OH center dot 2CH(3)-CN center dot 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.