Here we report a chemical-free, simple, and novel method in which a part from a silver-based anode is controllably used in a straightforward manner to produce silver nanoparticles (Ag NPs) in order to fabricate a controlled assembly of Ag NPs and single walled carbon nanotube (SWCNT) hybrid structures. The attachment and distribution of Ag NPs along SWCNTs have been investigated and characterized by field emission scanning electron microscopy (FESEM). We have achieved the decoration of SWCNTs with different densities of Ag NPs by changing the deposition time, the applied voltage, and the location of carbon nanotubes with respect to the anode. At low voltage, single silver nanoparticle is successfully attached at the open ends of SWCNTs whereas at high voltage, intermediate and full coverage densities of Ag NPs are observed. As voltage is further increased, fractals of Ag NPs along SWCNTs are observed. In addition, a device based on a Ag NPs-SWNT hybrid structure is used for the label-free detection of ssDNA molecules immobilized on it. We believe that the proposed method can be used to decorate and/or assemble metal nanoparticles or fractal patterns along SWCNTs with different novel metals such as gold, silver, and copper and can be exploited in various sensitive applications for fundamental research and nanotechnology.