A new hydroxymethyl terminated pyrimidine-hydrazone (pym-hyz) ligand (L1) was synthesized with a central hyz-pyridine-hyz (hyz-py-hyz) motif replacing the usual hyz-pym-hyz unit, to create a molecular strand that underwent metal-induced isomerization with a minimal net change in ligand length. NMR spectroscopy showed that L1 had a horseshoe shape due to the hyz-py-hyz and pym-hyz bonds adopting transoid conformations. The ligand was successfully reacted with Pb(II), Zn(II), and Ag(I) salts in either CH3CN or CH3NO2 resulting in horseshoe-shaped M(3)(n+)L1A(3n) (where A = ClO4- or SO3CF3-) complexes in the solution phase. Crystals were grown from these solutions, the structures of which were highly dependent on the metal ion and solvent used, and were distinctly different from those seen in solution. The crystals grown from mixtures of Pb(ClO4)(2)center dot 3H(2)O and L1 in either CH3CN or CH3NO2 resulted in the horseshoe-shaped [Pb(3)L1(ClO4)(4)(H2O)(2)}(ClO4)(2). CH3CN (1) complex or the {[Pb(3)L1(ClO4)(4)(H2O)}(ClO4)(2)}(infinity)center dot CH3NO2 (2) helical coordination polymer, respectively. The horseshoe-shaped [Pb(3)L1(SO3CF3)(6)]center dot CH3CN (3) complex was crystallized from a solution of Pb(SO3CF3)(2)center dot H2O and L1 in CH3CN, while the crystals grown from the solution of Zn(SO3CF3)(2) and L1 in CH3CN consisted of the zigzag-shaped [Zn(3)L1(H2O)(7)](SO3CF3)(6) (4) complex. The [Ag-3(L1)(2)](SO3CF3)(3) (5) double-helicate and the macrocycle-like [Ag-6(L1)(2)]-(SO3CF3)(6) (6) complex were crystallized from solutions of AgSO3CF3 and L1 in either CH3CN or CH3NO2, respectively.