Binary nanostructure array,in which the sub-component arrays are made of two (or more) different materials or structures in one unit,has been demonstrated to be an innovative principle for designing and constructing functional devices and systems [1-5].In particular,when the binary sub-components are at the interplay distance,intimate coupling between the two components becomes dominant and endows the macroscopic materials with novel properties and superior functionalities that cannot be achieved by either of the building blocks.In order to qualitatively disentangle the interplay between the building blocks,different strategies,such as ottom-upchemical processes and opdownphysical approaches,have recently been explored.However,these strategies have limited compositional and morphological options,and the resultant binary nanocrystal superlattices and nanodots have poor uniformity and distribution.