There are various fabrication methods for synthesizing nanostructures, among which plasma-based technology is strongly competitive in terms of its flexibility and friendly uses, economy, and safety. This review systematically discusses plasma techniques and the detailed interactions of charged particles, radicals, and electrons with substrate materials of, in particular, polymers for their nanostructuring. Applications employing a plasma-based nanostructuring process are explored to show the advantages and benefits that plasma treatment brings to many topical and traditional issues, and are specifically related to wettability, healthcare, or energy researches. A short perspective is also presented on strategic plans for overcoming the limitations in dimension from surface to bulk, lifetime of surface functions, and selectivity for interactions.