The Surface Nanoscale Kirkendall Effect is an important part of the Kirkendall effect, and has special role in the formation of surface nano material configurations. It can also cause faults in interconnection contact systems, yet this kind of effect has not yet been identified and studied in detail. Based on the obtained experimental results, this paper proposes a formation mechanism and model of the mixed-surface nanoscale Kirkendall effect formed by the role of Au metal catalyst islands/strips on a GaAs surface using the thermal Vapor-Liquid-Solid method. The diffusion of Ga, As, O atoms and the absorption of O atoms from a low-vacuum ambient into Au droplets forming surface nanoscale Au/Ga/O clusters leaves behind vacancies and voids; this process results in the nanoscale Kirkendall effect. In addition, the outward diffusion of the surface nanoscale Au/Ga/O clusters leaving behind bare GaAs holes in place of the former Au island forms the surface Kirkendall effect. Consequently, the combination of the two mentioned effects forms a new kind of KE, the so-called Surface Nanoscale Kirkendall Effect. This effect is generated either partly or completely, depending on the technological conditions. Accompanying this effect, the different configurations of nanomaterials have grown in number. The outward diffusion of surface nanoscale Au/Ga/O clusters was caused by the concentration of surface cluster gradients, the weakening of chemical bonds due to the accumulation of vacancies, the porosity, and pit-etching beneath the Au island. The diffusivity of surface Au/Ga/O clusters is numerically estimated. Its values vary from 2 × 10−10 to 10−11 m2/s. Potential applications of the surface nanoscale Kirkendall effect, making use of its advantages, limitations and disadvantages, are also discussed and proposed.