Approaching micro-world applications there is the need for a precise tailoring of the physico-chemical properties and functionalities of smart materials and often the demand for their adaptability to different work conditions and processing techniques. Smart polymers, with their almost infinite capability to be modified for the precise “tuning” of desired properties and with their generally easier and cheaper processing, seems to be well suited as candidates for the development of smart microstructured actuation systems. Respect to their inorganic counterpart (metals, alloys, ceramics, crystals) polymers indeed permit a wider freedom in setting and modifying synthetic procedures; they could be quite easily processed together with other organic/inorganic/biological compounds in order to develop functional blends, hybrid composites and nanocomposites; micro and nanopatterning of polymers, with resolutions down to 100 nm or lower, is nowadays available with relatively inexpensive techniques such as hot embossing and imprinting or also exploiting self-assembling procedures and supramolecular arrangement of organic molecules. In this way novel “soft” nanofabrication processes, very different from more common lithographic techniques, are exploited for the production of nanostructured organic materials such as nanostructured polymer gels and polymer brushes that open the way towards nanoactuation. In addition, post-modification of polymer surfaces, in order to include specific functionalities on existing surfaces to e.g. induce change in wettability properties or alter biomolecular functions, is quite easily achieved by chemical modifications. Moreover the deposition of thin layers of polymers is easily prepared with techniques as spin coating that are faster and cheaper than those required for deposition of thin layers of inorganic counterparts and that are very often performed under high-vacuum conditions.