We began by exploring the impact of varying the strength of attraction 𝜀 ?@ between the cores of NPs. Note that this interaction between NP cores does not appear in the three-body interaction, so tuning 𝜀 ?@ will only affect the pairwise two-body interactions 𝑊 ! . Even here, changes in 𝜀 ?@ will simply shift 𝑊 ! (𝑑) relative to the one we computed for 𝜀 ?@ = 30𝜀 by an amount equal to the difference in the new and original attractive core-core potential 𝑈 GG , that is, 𝑊 ! (𝑑; 𝜀 ?@ ) = 𝑊 ! (𝑑; 30𝜀) + 𝑈 GG (𝑑; 𝜀 ?@ ) -𝑈 GG (𝑑; 30𝜀), which can be rapidly calculated. When we reduced the vdW attraction to 𝜀 ?@ = 20𝜀, the previously obtained 2D sheets could not be realized, and NPs instead assembled into a loose network of NP strings (Fig. ). The reason is that the weaker core-core attraction leads to a weaker two-body attraction between NPs, making the three-body repulsion relatively stronger. This repulsion is now too strong to support the assembly of 2D sheets, but not strong enough to promote assembly of 1D strings, causing the formation of a structure intermediate to the two. On the other hand, increasing the attraction to 𝜀 ?@ = 40𝜀 led to the formation of small 3D NP clusters that remain stable in size even over a very long timescale of 𝑡 = 4 × 10 F (𝑚𝜎 ! 𝜀 ⁄ ) 4/! (Fig. ). Interestingly, while the stronger two-body attraction should promote continuous merger of clusters until a single globular aggregate remains (Fig. ), the three-body repulsion seems to prevent cluster aggregation. This is likely because the many triads of three-body repulsions arising from the NPs in the clusters create energy barriers between each cluster that prevents them from further aggregating.