Chemical vapor deposition (CVD) is a widely-used technology for the preparation of conformal and defect-free inorganic thin films with systematically tunable properties. Polymers are a desirable class of materials for surface modification because of their low cost, wide array of chemical and physical functionality and mechanical flexibility. Initiated and oxidative chemical vapor deposition (iCVD and oCVD) are polymer CVD methods that combine the benefits of CVD processing with the possibilities of polymeric materials. Using these technologies, our laboratory has synthesized a number of functional, biocompatible and electrically conducting polymers as thin films on micro- and nano-structured surfaces. This Perspective will review recent advances in these areas and highlight devices and applications that utilize iCVD and oCVD polymers.