This study investigates carbon-nitrogen thin films as active materials in photocatalytic methanol reforming, addressing the need for eco-friendly fuels with minimal waste and non-metallic photocatalysts. Additionally, it explores the synthesis of these materials using plasma-enhanced chemical vapor deposition (PECVD) from acrylonitrile or acetonitrile. This area has limited prior attention in carbon-nitrogen materials synthesis, particularly with subsequent application in methanol reforming offering potential advancements in clean energy production. The aim is to develop effective, environmentally friendly sources of hydrogen, where photocatalysts play a crucial role. The studies involved also characterization for morphology, and chemical structure. The results confirmed the activity in hydrogen production through methanol reforming, achieving a promising rate of 82 ± 6 μmol h−1 cm−2.