Self-assembled monolayers (SAMs) are good candidates for electronic molecular devices as they are compatible with fl exible substrates, show reliable fi lm-forming behavior, fi t well with the miniaturization concept and can be easily functionalized by changing the constituent molecular components. [ 1 ] Most studies on the electrical properties of SAMs have focused on the conduction along the molecular axis [ 2 ] even though this is a minor aspect of the electrical transport in SAMs as they are inherently intended to operate through lateral charge transport which instead depends strongly on intermolecular packing. [ 3 ] Several approaches, [ 4 ] some of which are outlined in Figure 1 , have been proposed to study the lateral electrical transport in SAMs. Field-effect transistor devices in which the semiconductor channel is a single sheet of molecules formed on the gate dielectric (SAMFETs, Figure 1 a) are the most common approach and allow the charge carrier mobility to be extracted from the fi eld-dependence of the source-drain current. [ 5 ] In the case of SAMs formed on conductive substrates, the dependence of the domain height on the size of isolated molecular islands as measured by scanning tunneling microscopy (STM, Figure 1 b) provides an indirect assay of intermolecular charge transport between neighboring molecules. [ 6 ] However, these techniques disagree widely on the magnitude and mechanism of charge transport in monolayers, which can range from very high mobility through ballistic charge transport [ 5 ] to low-to-moderate mobility via percolation. [ 7 ] To date, direct probing of the conductivity of a single molecule layer has not been possible due to the diffi culty of achieving good electrical contact without damaging the monolayer and the low currents that are expected in the absence of a fi eld-effect. In this respect, conducting atomic force microscopy (C-AFM, Figure 1 c), is particularly well adapted as the combination of AFM imaging and C-AFM electrical characterization enables separate (in contrast to STM) and simultaneous (in contrast to SAMFETs) investigation of the structure and function of molecular assemblies. [ 2c ] In addition, C-AFM can be used to measure samples with widely varying conductance, while positioning an electrical probe with nanometer scale precision and controlled force, [ 8 ] thus enabling the channel length to be varied in a step-wise fashion down to tens of nanometers. [ 2c ] Several groups have successfully used this technique to study electrical transport in surface-confi ned nanostructures such as semiconductor crystals, [ 8,9 ] DNA molecules, [ 10 ] inorganic [ 11 ] and organic [ 12 ] nanowires, and carbon nanotubes. [ 13 ] However, initial attempts to measure the lateral transport in SAMs using C-AFM were unsuccessful and the weak currents observed were attributed to tunneling between the tip and the fi xed electrode. [ 14 ] Achieving good contact between a monolayer and a metal electrode is critical for electrical measurements. The evaporation of a ...