As clinical neuromodulation moves beyond electrical stimulation with macroelectrodes, the need becomes apparent for techniques that interact with the nervous system on its own level (neurons and glia) and using its own mechanisms (electrical and chemical). To communicate in a manner that corrects nervous system disorders (rather than merely masking them) requires techniques at the micron to submicron (cellular and possibly intracellular) level. Substituting appropriately configured carbon nanoelectrodes for platinum macroelectrodes affords orders of magnitude improvement in both charge transfer (stimulation) and charge detection (recording). Nanoelectrodes offer the ability to monitor, simultaneously, several neurotransmitters in real time as well as electrical activity. To take full advantage of the possibilities of micron-level nanoarrays for neuromodulation, two techniques will need to be incorporated: (1) computational modeling of both nervous system electrical and chemical activity and (2) minimally invasive access to all regions of the nervous system.