As a second complex hierarchical structure, we investigated the formation of colloidal "alloys" obtained in a single step. We took advantage of the gravity-dependent accumulation of particles to the drop centre to partition particles of different sizes dispersed in the same drop, co-crystallize them, and deposit the resulting structure on the solid substrate (Fig. ). Figure shows a typical deposit obtained drying a drop containing a mixture of 2.4 μm and 560 nm silica particles (Vdrop = 5 μL, Cs = 10 μM, Cp = 0.1 mg/mL and Cp = 0.05 mg/mL for 2.4 μm and 560 nm particles, respectively). The particles with the bigger diameter sedimented and slid down the curved interface faster than the smaller ones, and gathered at the centre of the assembly where they crystallized (Fig. ). Only few small particles were trapped in the interstices of the close-packed hexagonal lattice, without perturbing the long-range order. Instead, the smaller particles accumulated at the periphery of the central crystal and further crystallized in the outer region (Fig. middle). The transition between the two lattices was characterized by a disordered accumulation of the smaller particles and a higher density of the interstitial particles in the larger lattice. Interestingly, a band of large particles was also observed at the outer rim of the deposit (Fig. , opposite to what is obtained when drying mixtures of particles from drops in sessile configuration. This peculiar size-sorting might be due to the capillary trapping of few particles at the contact line which were eventually merged to the assembly at the last stage of evaporation. By increasing the drop volume (Figs. 5d, S11), or by varying the concentration ratio in the mixed dispersion (Fig. ), phase-separated colloidal alloys of different sizes were obtained in a well-controlled manner. For example, a decrease in the concentration of small particles (small-to-big mass ratio of ¼ instead of ½) led to a specific decrease of the outer crystal area, keeping the size of the inner crystal unmodified (red marks in Fig. ). This demonstrates how ordered assemblies of particles with different diameters could be conveniently obtained in a direct manner exploiting gravity-controlled size-sorting at a fluid interface. Last, benefiting from the strong adsorption of particles at the liquid interface, we adapted our deposition method to obtain 2D colloidal "irises", i.e. rings of crystalline monolayer with a particle-free centre. We first deposited on the substrate a drop of the colloidal dispersion, flipped it upside-down to let particles adsorb at the a/w interface and accumulate at the centre of the drop for approx. 1 h. The drop was then flipped again and left drying in sessile configuration for an additional hour (Fig. ). When the drop was upside-down, particles assembled into a disk-like 2D crystal, but after flipping to sessile configuration, the particles remained trapped at the a/w interface and rapidly slid down toward the rim of the drop (Fig. , Movie S7). Pre-assembled large crystalline domains were redispersed into smaller cluster by convective surface flows and progressively recrystallized during the final stage of evaporation (Movie S7). At fixed drop volume (Vdrop = 5 µL), the final deposit was dependent on the particle concentration, resulting in the formation of different structures as a function of Np (Fig. ). When the particle concentration was too low (Cp = 0.01 mg/mL), the few particles at the interface were not dense enough to collectively crystallize prior to their deposition, therefore forming a ring-shaped deposit but with no long-range order and only small hexagonally-packed clusters (Fig. ). In contrast, a well-organized polycrystalline iris was obtained for intermediate particle concentration (Cp = 0.05 mg/mL, Fig. ). In that case, particles were in sufficient amount to crystallize from the drop rim after the second flipping, but could not cover the entire a/w interface, therefore splitting into a ring and leaving an empty central region when depositing on the substrate. Finally, for a larger particle concentration (Cp = 0.1 mg/mL), a large disk-like assembly could be formed at the drop a/w interface both before and after the second flipping and it was thus deposited as a whole layer (Fig. ), in a way similar to the one obtained by drying drops in hanging configuration. Exploiting its simple format, the hanging drop deposition of ordered colloidal monolayer was thus shown to be easily evolvable to more elaborate deposition protocols allowing the controlled deposition of complex colloidal assemblies, ranging from orientation-independent monolayers assembly to crystal alloys and polycrystalline irises.