Despite the approximations in our CG molecular model (necessary to simulate the relevant space-and time-scales for an exhaustive characterization of the collective mechanisms underpinning the supramolecular conductive process), even from a purely qualitative standpoint our simulations clearly demonstrate how the classical interactions involved in colloidal supercrystals can give rise to complex emergent charge transport behaviors, with nonlinear dependence of the material resistivity on the variable external stimulus. In particular, the non-ohmic behavior demonstrated in Figures , and 5 indicates that the nonconductive/conductive transition is related to the fact that an activation free energy barrier must be overcome to the conduction processi.e., breaking the electrostatic NP-CIT interactions to release CIT ions for conduction. The presented approach can be applied to study and rationalize the ionic conductive properties in different kinds of colloidal supercrystals; this study thus demonstrates how binary conductive properties, which are at the basis of fundamental logic applications in semiconductors, can in principle emerge also in supramolecular systems ruled by non-bonded interactions. Our results provide an explicit example of how a supramolecular material may indeed present semiconductive or metallic-like behaviors, even on a higher scale. These results also greatly improve our understanding of how, in such complex molecular systems, concerted dynamics and stimuli-responsive ensemble properties may emerge from collective molecular behaviors in a way that can be understood only by studying the effect of the stimulus on large ensembles of discrete individual entities.