Clusters are well-known molecular units with atomically precise structures, which are characterized by their subnanometer scale and fascinating properties that offer a variety of functions. The ability to manipulate self assembly using solvents is crucial for precise nanostructure fabrication. Herein, we report a novel strategy to fabricate nanostructures with multiple dimensions (0-3) via the principles of lipid self-assembly. First, we designed and synthesized a truncated cone heterocluster Janus molecular building block comprising two types of clusters, viz. polyoxometalate (POM) and polyhedral oligomeric silsesquioxane (POSS), which are covalently bound via an organic linker (OL). A variety of nanostructures was obtained by adjusting the solvent polarity, hydrogen bonding, and dispersion forces. Finally, we explored the relationship between the solubility parameter of solvents and nanostructures, providing a systematic study of self-assembled nanostructures manipulated in different solvents. These ordered nanostructures can serve as an ideal structural component to fill the gap in the size range between inorganic crystals and nanoparticle supracrystals, which is of significant importance in the design and development of next-generation nanodevices.