Structural diversity and uniformity of nanomaterials are usually prerequisites for many practical applications involving the oriented fabrication of various devices with full control over their desired physiochemical properties. Particularly in the optoelectronic field, ordered assembly inside cells is required not only for obtaining attractive configurations but also for playing an important role in the characteristics of photoconduction and conductivity. Here, we present a synergetic self-assembly driven by coordination and intermolecular interactions for the construction of organic-inorganic hybrids with multi-morphologies and tunable physical properties. 3,4,9,10-Perylenetetracarboxylic dianhydride was treated with base to produce various assemblies by coordination with metal ions, showing morphologies of nanowires, nanosheets, nanoribbons and nanorods. The organic π-spacer affords an extension in different directions through the suitable incorporation of metal ions with different coordination modes for the formation of metal-ligand complexes. Interestingly, the obtained nanorods were twisted rods with obvious screw threads on the rod wall, supporting the synergetic self-assembly. Then, anisotropic mobility measurements of the obtained Cu(2+)-ligand assembly were carried out to show the importance of the size- and shape-confined synthesis of the hybrids. By presenting a series of ordered metal-ligand complex superstructures driven by synergetic self-assembly, this work is expected to pave the way for future anisotropic measurements of complex assemblies.