The evolution of complex morphologies requires control over the synthetic parameters such as solvents, temperature and additives. Different mechanisms have been proposed for the formation of sheaf-like and spherulites superstructures, including (i) crystal splitting and (ii) non-crystallographic branching. Anisotropic sheaf-like structures are intermediates in the formation of spherulites. The former mechanism (i) results in splitting of a parent crystal (= simple splitting) and the structures develop into rods or lamellas at the tips resulting in hedrites, sheafs, and spherulites. The latter process (ii) termed non-crystallographic branching was postulated by Keith and Padden and is believed to involve secondary nucleation of crystals on a seed with a slight misorientation. We found only a few literature reports on metal-organic frameworks (MOFs) with sheaf-like and spherulite shapes. You and Han et al reported such shaped MOFs and coordination polymers based on lanthanides as metal ion centers and benzenetricarboxylate (1,3,5-BTC) as coordinating ligand. These materials exhibit tunable light emission. Another recent example is the spherulite MOF-74 reported by Zhou et al formed via small-angle branching and radial growth. The spherulite MOF-74 has a fused core and surface fibers. Under polarized light, these crystals exhibit a solvent-dependent Maltese cross pattern as is common for spherulites. The paucity of examples of sheaf and spherulite shaped MOFs is surprising. Coordination chemistry has been extensively used for the formation of numerous MOFs during the past decades. These crystalline structures are explored for energy storage, carbon capture, catalysis, etc. MOFs are also promising materials for optical applications. Adsorption of dyes into their voids resulted in nonlinear optical and fluorescence properties, and Förster resonance energy transfer (FRET). The alignment of dyes in nanosized channels resulted in optical anisotropy. Their properties can be tuned by using different metal centers and organic linkers. Although great progress has been made in the control of packing, network structures, and porosity; the control over the morphology and uniformity of such useful crystals remains an intriguing challenge. The formation of new hyperbranched MOFs can lead to new functionalities as shown in this study. Our group has recently shown that the coordination chemistry of tetrahedral pyridine-based ligands with first row, bivalent metals (i.e., nickel and copper) resulted in uniform structures. These studies include the preparation of rare single crystals having multidomain morphologies. Until now, we have not observed hedrites, sheaf and spherulite superstructures with our pyridine-based ligands.