The main research efforts of our group focus on the fabrication of functional nanomaterials by assembling nanobuilding blocks into designed patterns. The nanobuilding blocks that we employ range from nanospheres of polymeric latexes or metal oxides to amphiphilic molecules such as surfactants and block copolymers. To create all best-performing materials requires the precise control of their microstructures. During the last decade in our group, we have developed a general framework for predicting the self-assembled microstructures of nanobuilding blocks under equilibrium and nonequilibrium conditions. A variety of the fabrication strategies for designed microstructures have been undertaken utilizing soft microfluidic devices, electrohydrodynamic atomization, capillary interactions, holographic lithography, multiphoton absorption polymerization and DNAs (or proteins) as linker molecules. The designed nanostructures create unusual fascinating multifunctions.