This work reports for the first time electrosynthesis of hexanethiol capped silver nanotriangles cores (Ag@C6SH NCs) by a rapid, clean, and simple Double Pulse Chronopotentiometric (DCP) method in nonaqueous media, using a Taguchi orthogonal arrayL8design to identify the optimized experimental conditions. It was found that the size and shape of the product could be tuned by the current density, electrolysis time, electrode distance, and amount of NaBH4% used. The Ag@C6SH NCs in different shapes and sizes (in the range of 30 to 44 nm as an average estimation) were synthesized, under different experimental conditions. Finally, the as-prepared nanoclusters electrosynthesized at optimized conditions were characterized by SEM, XRD, and UV-Vis spectroscopy. The average particle size of the triangular/pyramidal shape (Ag@C6SH NCs), obtained under optimized experimental conditions, was30.5±2.0 nm but the majority of nanoparticles in TC3SEM are so much finer.