This work focuses mainly on the influence of time, temperature, and contact with food simulants on the adhesion of amorphous hydrogenated carbon (a-C:H) films obtained by plasma-enhanced chemical vapor deposition (PECVD) in clarified polypropylene (cPP). Two types of films prepared by PECVD were studied: diamond-like carbon (DLC) and polymer-like carbon (PLC) films that can both act as a functional barrier. The adhesion between the film and polymer substrates is critical in relation to the barrier effectiveness during the packaging shelf life. Therefore, the adhesion was analyzed by a tape test and scanning electron microscopy (SEM). The films were exposed to Food and Drug Administration (FDA) listed food simulants and were submitted to an accelerated aging test to evaluate the long-term adhesion performance of a-C:H films. The chemical alterations on the surface related to the accelerated aging test and the liquid simulants were analyzed by a contact angle test. It showed that the polarity of a-C:H films increased after immersion in liquid simulants, indicating a change on the surface. Before the accelerated aging test, the SEM micrographs and the tape test indicated that the PLC film has a structure with lower surface tension and, therefore, regions with fewer detachment points in relation to the DLC film. The results obtained in this study showed that the adhesion behavior and preservation of the a-C:H structure (DLC or PLC) are related to intrinsic factors such as the type of film structure (flexible or rigid) and the polymeric substrate.