Two complexes, 2D [Cu(2)(CN)(2)(4-Hpcih)](n) and 3D [[Cu(2)(CN)(1.5)(4-pcih)].1.25H(2)O](n) (4-Hpcih = 4-pyridinecarbaldehyde isonicotinoyl hydrazone), were obtained using a synthetic approach of pH-induced formation of metalloligands, successfully demonstrating a strategy to increase structure dimensionality by tuning the number of ligand functional sites.