Large, polarizable systems require accurate treatment of non-local electronic correlations, such as van der Waals (vdW) dispersion, which affects both energies and ρ(r) (and related properties). Nevertheless, most of the popular vdW methods, such as the DFT-D family by Grimme et al. or exchange-hole dipole moment (XDM) model of Johnson and co-workers , treat vdW dispersion as a posteriori energy correction without accounting for the resulting vdW polarization of ρ(r). While this may be sufficient for small molecules, it becomes inadequate for larger, more polarizable sys-tems, where dispersion-driven stabilization is significant . Recent studies suggest that vdW interactions can induce substantial polarization in ρ(r) for complex systems, e.g. π-stacked supramolecular dimers or molecules on a surface , but a comprehensive assessment of the relative role of vdW-induced ρ(r) polarization in comparison to semi-local (or hybrid) DFAs remains lacking.