The weaker solvent structure close to the NP is not a general feature of hydrophilic NPs, instead, it is a consequence of the interaction parameters employed. Increasing the interaction between hydrophilic NPs sites and the anion by 50% leads to the distributions and structures shown in Figure in Supporting Information file, which displays peaks with similar intensity displayed by the hydrophobic NP, but with the first layer rich in anions instead. This change in the interaction parameters, although arbitrary in the simulation, could correspond to a change in either the NP material or in the IL anion, and is more likely to reproduce a metallic NP than the parameters employed for the hydrophilic NP for the rest of this work since metallic NPs tends to interact preferentially with the anion of ILs. If the pmf was computed for the NP of Figure , a higher activation barrier would be observed for the hydrophilic NPs in C4. The "weaker" or "stronger" structure of a given IL close to a NP is not necessarily a consequence of the hydrophilic or hydrophobic nature, but instead of the relative intensity of the interaction of the NP with specific groups of the IL in relation to their interactions inside the IL.