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Nanostructured materials with optical properties responsive to external stimuli are gaining increasing interests due to their intrigue potential applications in printing, sensing, signage, security documents, displays, and other color related devices. In this presentation, I will first discuss our recent progresses on the development of chemical approaches for the fabrication of various nanostructured materials whose optical properties can be dynamically tuned by controlling the spatial arrangement of the nanoscale building blocks.[1-3]