Abstract Graphene is a promising material for membrane applications. However, the graphene production with large specific area and good structural quality is a challenge. Therefore, the production and characterization of composite membranes with graphene grown by chemical vapor deposition (CVD) over a porous polymethylmethacrylate (PMMA) substrate was investigated. The experimental strategy consisted in applying CVD‐graphene on a PMMA surface using PMMA‐assisted graphene wet transfer. The proposed methodology resulted in large‐area membranes with 2 cm diameter. The samples were characterized by Raman spectroscopy, indicating the presence of graphene in good quality and relative structural integrity. The analysis by scanning electron microscopy revealed the formation of a microporous support with an asymmetric structure. The gas permeation measurements of graphene/PMMA membranes showed a permeability reduction of 81.9 for CO2 and 83.7 for N2. The contribution of PMMA to flow resistance was 2 and 11 for CO2 and N2, respectively, and the contribution of graphene was 98 and 89 for CO2 and N2. Therefore, this research presents a potential advance in transferring graphene to porous support, and the impermeability process of membranes composed of graphene/PMMA, a fundamental step for the development of graphene membranes before the production of controlled‐sized pores.
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