Molecular modulators have been used by others to control crystal morphology and dimensions. In this system, the components themselves act as modulators by shaping the appearance and dimensions of their architecture at the microscale while keeping their molecular arrangement nearly identical. These morphologies depend not only on the metal cations used, but also on the metal salt-to-ligand ratio. Decreasing the Cu 2+ concentration resulted in a series of different structures resembling flower-like morphologies. The fascinating double-decker flower-like morphology has a sixfold (C6) and twofold (C2) axis of symmetry perpendicular to each other. The high level of symmetry indicates that the growth rate for each sub-unit of the double-decker crystals is very similar. This study revealed that the nature of the first-row metal salts controls the crystal growth with our tetrahedral polypyridyl ligand, and hence the morphology, while maintaining a similar crystallographic packing with hexagonal space group P622. We have previously reported on stellate and chiral crystals grown from related ligand systems. Interestingly, Cheul Cho et al. recently reported the co-crystals of C60 and C70, which have similarly shaped double-decker flowers. The observation that completely different types of materials may crystallize in highly unusual double-decker flower morphologies indicates that this crystal shape may be a general phenomenon, with the expectation that additional examples remain to be discovered.