Carbon nanotubes have received attention as alternative materials to indium tin oxide for application in transparent conductive films. Their electrical conductivity, however, still has to be improved. In this study, a layer-by-layer self-assembly process was demonstrated using nano-silver-coated carbon nanotubes, which help improve electrical conductivity. The method was based on the pi-pi interaction between the side walls of the carbon nanotubes and nano-silver clusters that were functionalized with benzyl mercaptan. The self-assembled nano-silver cluster monolayer on the surface of the nanotubes can reduce the interfacial contact resistance, thereby leading to high conductivity at a high transparency. The compound was characterized via scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), Raman spectroscopy, and the four-point probe method.