It is worth remarking that this mechanism, illustrated above as a step-by-step kinetic process, also reflects the thermodynamic stability of the final aggregate topology. To prove this concept, we designed 6 additional simulations in which the starting configuration of each system has been set to a different, "non native" topology (chains and ribbons for allMUS, dumbbells and ribbons for MUS:OT 2:1, dumbbells and chains for MUS:OT 1:1). As better detailed in the SI (Figure ), in each of this artificial systems the starting topology was not stable and evolved towards the "native" one. As detailed in the SI, the NP reshaping upon aggregation can be quantified by its asphericity in the final aggregate. When NPs are isolated, the NP-water interface is roughly a sphere, and the average asphericity is 0 for any ligand composition. When NPs aggregate, instead, their shell is deformed, and the asphericity increases. In Figure , we report the NP asphericity β obtained in each system from the final aggregate of 27 NPs and measured as an average over each NP and trajectory. The Eventually we remark that the anisotropic structures observed in this computational study are coherent with experimental observations in similar systems. In a past work, different aggregate topologies (characterized by a different coordination numbers) have been experimentally obtained and interpreted in terms of ligand migration and rearrangement on the surface of the gold nanoparticles. However, the evolution of the shell morphology at room temperature, in absence of exchange reactions with ligands in solution, has been later reported to be very slow. Here we have shown that both the limited coordination number and the directionality of the interactions can originate from the soft NP shell reshaping due to aggregation, without any need for ligand migration.