A new approach to permanent hydrophilic modification of material surfaces is demonstrated using the deposition of nanoscaled functional coatings in RF plasmas at low temperatures under rivaling deposition/etching conditions. The incorporation of nitrogen and the generation of free radicals in a‐C:H films yields a strong hydrophilic modification when the deposited surface is exposed to atmosphere. Dyeing of nanoporous a‐C:H:N films demonstrated a high coating quality and the incorporation of accessible amine functionalities within the coating. This combination of polar groups with a suitable texturing ensures long‐term mechanical stability of the coating.