The surfaces of materials are drastically different from their bulk. Due to large surface-to-bulk ratios, surface properties play a dominant role in determining the overall properties of nanomaterials. Understanding and control of surface structures are essential to tailoring nanostructures and their applications. The project aims at studying, controlling, and manipulating the structure and properties of single nano-objects based on the concept that any nanomaterials are essentially a core-shell structure with properties largely determined by the shell. The outcome of the project may lead to various novel nanostructured devices for renewable energy, sensors for food safety, toxins and diseases, targeted drug releases.