As children play with wooden building blocks, we would like to construct elaborate architectures through the one-by-one accumulation of nanocrystals. Recently, ordered microarrays of nanosized building blocks have attracted attention as a sophisticated bottom-up approach to fabricate adequate nanomaterials. However, their dimensions, scale, and orientations have not been strictly controlled. The present highlight article reports the potential of brickwork structures using evaporation-driven manipulation as a nanoscale architectural method. Here, the essence of controlled assembly is shown with a demonstration of 1D, 2D, and 3D brickwork structures designed with various inorganic rectangular building nanoblocks covered by stabilizing organic agents. The structures of the ordered assemblies are found to be controlled by changing several parameters, such as particle concentration and the properties of dispersion media and stabilizing agents. This brickwork technique is applicable to multicomponent systems using a library of rectangular nanoblocks. Homogeneous and heterogeneous ordered architectures with spatial and sequential control are selectively produced through the self-assembly of nanocubes and nanocuboids. These elaborate nanoscale brickwork structures are now being developed for the production of designed microstructures with novel functions.