After infiltrating the deposited SPs with an epoxy thermoset, a composite material with two hierarchical levels (HLs) is obtained (Fig. ). Here, a cylindrical polyethylene mold was used in order to obtain macroscopic, disc shaped geometries. It is noteworthy that the used molding process can also handle other complex-shaped templates, allowing to obtain macroscale shapes tailored to the final application. The supercrystalline structure of the secondary building blocks (SPs) was maintained after infiltration, as confirmed by the fracture surface micrograph (Fig. ) and SAXS diffraction pattern in Fig. . An increase in the interparticle distance up to 1.8 ± 0.1 nm (from the original ca. 1.3 nm) was observed after infiltration, which can be explained by liquid epoxy resin precursors infiltrating the NC-NC interface at the 1st HL. A relatively dense packing of the 2HL structures could be achieved, leading to a low organic content of 16.7 ± 1.7 wt% epoxy resin in the final 2HL material, as obtained via thermogravimetric analysis (Fig. and, more information in the Methods section).