During the last decades, the possibility to establish a bidirectional communication link with electrically excitable cells, such as neurons, has become very attractive for both fundamental and medical purposes. Many conceptual and technological advances have been achieved, including in the field of neuroelectronics, which remains a unique way to obtain quantitative measurements of neuronal electrical activity and tailor specific stimulations. In addition to recording the activity of many neurons individually, electrical devices are indeed able to stimulate or inhibit neural spikes at single-cell level within large networks, which makes them suitable tools to interrogate neural networks within the brain, [1] in slices or cell cultures. [2] With nearly 40 years of development in that field, numerous materials and designs have been implemented on many substrates, including transparent or flexible planar and 3D electrodes, [3][4][5][6] but still the current conventional microelectrodes (MEs) face limitations to reach the ultimate sensitivity and to probe subcellular events such as ion channel, dendrite, or