Organic materials can exhibit responsive behavior, including swelling upon exposure to a specific chemical analyte or displaying a switch surface energy in response to a change to external stimuli. The initiated Chemical Vapor Deposition (iCVD) of responsive surfaces facilitates their integration into novel devices and into roll-to-roll processing. Incorporating responsive organic layers into devices creates the ability to transduce chemical or biological events into optoelectronic signals. Additionally, ultrathin, responsive layers enable the design of novel membranes for separation and purification. This work describes the ability to synthesize thermally responsive organic layers by initiated Chemical Vapor Deposition (iCVD). (C) 2011 Elsevier B.V. All rights reserved.