Next, we explored the flexibility of our method in achieving controlled colloidal deposition into more complex architectures, which can hardly be attained by common deposition strategies. First, we took advantage of the adhesion of the dried assemblies on the substrate to repeat the process and add monolayers on top of already formed ones, conveniently producing colloidal materials with structural hierarchies. The successive deposition of ordered particle layers was obtained by using the following experimental procedure: a first monolayer was assembled on the substrate as previously described, then a second drop of particle suspension was carefully placed on top of the already assembled pattern, the substrate was flipped down and kept in a closed chamber until complete evaporation (Fig. ). We first deposited either a drop containing 2.4 μm silica particles above an already formed layer of 2.4 μm particles (Fig. ), or a drop containing 560 nm particles above an already formed layer of 560 nm particles (Fig. ).