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Nanofabricated polymers are extremely useful due to their high functionalities caused by the inherent multiscale structures of the nanostructured polymers. Nanostructured polymers for biocoatings can be classified into zero-dimensional (0D) polymeric nanoparticles, 1D polymeric nanofibers, and 2D polymeric nanosheets. The nanostructured polymers with such different dimensions were most often fabricated by emulsion polymerization, electrospinning, and spin coating. To add a desirable and advanced functionality to the targeted nanostructured polymers, surface modifications of the polymers can be highly advantageous. The surface modifications such as plasma etching, plasma-induced cross-linking, plasma polymerization, and chemical vapor deposition can effectively modify the surface characteristics of the nanofabricated polymers, leading to the enhancement of the bulk physical properties of the polymers. In this chapter, the fabrication methods of such nanostructured polymers are reviewed. In addition, several successful cases of well-controlled surface conditions of polymers by plasma processing are introduced.