When NCs are directly assembled into bulk, 3D supercrystalline materials and crosslinked via heat-treatment without a multi-hierarchical design, severe cracking can be observed already at low indentation depths (Fig. ). Upon increasing the indentation depth, the bulk supercrystaks show a significant decrease in the measured elastic modulus and hardness from 32.7 ± 2.2 GPa down to 15.5 ± 1.1 GPa and 2.05 ± 0.19 GPa to 1.16 ± 0.19 GPa, respectively.