Understanding the mechanisms and controlling the possibilities of surface nanostructuring is of crucial interest from fundamental and practical perspectives. Here we report a direct experimental observation of laser-induced periodic surface structures (LIPSS) formed near a predesigned gold step edge following single-pulse femtosecond laser irradiation. A hybrid atomistic-continuum model fully supports experimental observations. We identify two key components of single-pulse LIPSS formation: excitation of surface plasmon polaritons and material reorganization. Our results lay the foundation towards simple and efficient single laser pulse micromachining.