Nanometre-scale roughness on a solid surface has significant effects on friction, since intersurface forces operate predominantly within a nanometre-scale gap distance in frictional contact. To study the effects of nanometre-scale roughness, two novel atomic force microscope friction experiments were conducted, each using a gold surface sliding against a flat mica surface as the representative friction system. In one of the experiments, a pillar-shaped single nano-asperity of gold was used to measure the molecular-level frictional behaviour. The adhesive friction stress was measured to be 264 MPa and the molecular friction factor 0.0108 for a direct gold-mica contact. The nano-asperity was flattened in contact, although its hardness at this length scale is estimated to be 3.68 GPa. It was found that such a high pressure could be reached with the help of condensed water capillary forces. In the second experiment, a micrometre-scale asperity with nanometrescale roughness exhibited a single-asperity-like response of friction. However, the apparent frictional stress, 40.5 MPa, fell well below the Hurtado-Kim model prediction of 208-245 MPa. In addition, the multiple nano-asperities were flattened during the frictional process, exhibiting load-and slip-history-dependent frictional behaviour.