Initially, ligands are straight and non-tilted. Using tilted structures from SAM simulations to construct sandwich structures unfortunately was not possible, as the cross-linkage in those sandwich structures was low (see Supporting Information, Section S2.3.1). We extract the average preferred surface-to-surface distances from 10 MD simulations where the surfaces are pushed together (see Section 2.1) and study the chain-length dependence of the preferred surface-to-surface distance. We compare our data with experimental data on cross-linked GNP assemblies. In addition, we analyze the atomistic structures and look into the fraction of bridging ligands and the presence of defects in the gold surface.