Structural control of nanomaterials is of paramount significance for nanodevice fabrication. This talk will highlight the concept, strategy, and scope of our recent works. We have so far demonstrated several basic concepts for the colloidal synthesis of complex nanostructures, for example, use of polymer shells as nano-capsules to protect the assembly of nanoparticles[3,4,6], development of methods for isolating high-purity dimers and trimers of nanoparticles[3,4]; use of polymer shells to break the symmetry of nanoparticles[2,5]; use of polymer shells to coil unltathin gold nanowires into circular rings; and development of colloidal “reactions” of nanoparticles. The novel nanostructures have provided useful insights in the studies of surface-enhanced Raman scattering (SERS) [3], drug delivery kinetics[1], and solid state growth[6,7]. The current focus is to impart specific functionalities to a judiciously designed nanostructure, where the different components could coordinate to achieve a certain function. Generally speaking, solution methods are facile, scalable, and reproducible. Our long-term goal is to emulate the synthetic methodologies of organic chemistry and fabricate nanodevices by multi-step colloidal self-assembly of nano-components.