Nanostructured particles (clusters) with complex and periodic topography at the microscopic scale show unique structural patterns. Hence, good properties should be obtained when the surface topography of such clusters, especially those containing nanoparticles (NPs) of different sizes, can be carefully tuned. The coffee-ring structure is one of the most interesting structures for catalyst and photonic crystal applications or porous particle molds. Here, well-defined clusters with a coffee-ring structure were prepared by spray drying. The complexity of the NP distribution in the resulting two-and three-component systems is discussed. A better understanding of how finite groups of different NPs self-organize in a moving droplet to form a confined geometry may aid in controlling the structure of matter at multiple length scales. Interestingly, the configuration of the large microsphere clusters was found to be influenced by the presence of the small particles, which formed a ring-like structure. (C) 2017 American Institute of Chemical Engineers AIChE J