New trends toward green technologies and broad utilization of polymers have led to intense research on surfaces with controlled wettability. This study demonstrates an easy method to control the wettability (estimated by static water contact angle [WCA]) of a polymer surface by introducing a proper ratio of C–F, C–H, and N–H bonds. The preparation method combines magnetron sputtering from a polytetrafluoroethylene (PTFE) target and plasma‐enhanced chemical vapor deposition (PECVD) from a nitrogen/acetylene mixture, making it environment‐friendly, unlike PECVD from hydrocarbons/fluorocarbons. The proposed method allows depositing plasma polymers with WCAs from 110° to 17° by varying only the gas composition. The corresponding plasma polymers consist of C:F (magnetron sputtering of PTFE), C:F:N:H (reactive magnetron sputtering and PECVD), and a‐C:H (PECVD from acetylene).