to batteries. [6] Additionally, it allows us to increase our understanding of molecular interactions in liquid, which is currently based on theoretical models of ensemble measurements. Towards these goals, scanning electrochemical microscopy (SECM), including the use of nanopipettes, [7][8][9] has been developed to sense electrochemical reactions locally, providing spatial resolution of typically μm to the sub-μm range, [10][11][12] but also fast reactions on nanometric particles could be resolved when well isolated. [13,14] SECM techniques are now well-established for probing electrochemical systems at the micro-and nanoscale levels. [15,16] Scanning probes have exploited redox-cycling amplification to reduce the electrode dimensions while keeping a reasonable signal level. [11,17,18] Electrochemical scanning tunneling microscopy (EC-STM) has been used to study electrochemistry indirectly from a molecular electronics perspective. [19,20] To date, these techniques have enabled measurements down to the fA (10 −15 Ampere) range, [11,[21][22][23][24][25] which is still not sensitive enough to obtain electrochemical signals at the nanoscale, except in the specific case of redox cycling amplification when ferrocene (Fc) is confined between 2 neighboring electrodes at the nanoscale. [23,25] For the versatile measurement of electrochemical currents at the nanoscale aA (10 −18 Ampere) sensitivity is crucial.Electrochemical microscopy techniques have extended the understanding of surface chemistry to the micrometer and even sub-micrometer level. However, fundamental questions related to charge transport at the solidelectrolyte interface, such as catalytic reactions or operation of individual ion channels, require improved spatial resolutions down to the nanoscale. A prerequisite for single-molecule electrochemical sensitivity is the reliable detection of a few electrons per second, that is, currents in the atto-Ampere (10 −18 A) range, 1000 times below today's electrochemical microscopes. This work reports local cyclic voltammetry (CV) measurements at the solid-liquid interface on ferrocene self-assembled monolayer (SAM) with sub-atto-Ampere sensitivity and simultaneous spatial resolution < 80 nm. Such sensitivity is obtained through measurements of the charging of the local faradaic interface capacitance at GHz frequencies. Nanometer-scale details of different molecular organizations with a 19% packing density difference are resolved, with an extremely small dispersion of the molecular electrical properties. This is predicted previously based on weak electrostatic interactions between neighboring redox molecules in a SAM configuration. These results open new perspectives for nano-electrochemistry like the study of quantum mechanical resonance in complex molecules and a wide range of applications from electrochemical catalysis to biophysics.