In this paper, a new synthesis of carbon‐based nanostructured films for application as plasma facing materials during high‐intense laser‐matter interaction experiments is presented. The materials are produced using a Polyethylene glycol (PEG) matrix, nanostructured with multiwalled carbon nanotubes, or multi‐layer graphene flakes producing a 250 μm thick film. The films are deposited onto typical materials used in harsh environments such as plasma facing materials. These PEG reinforced materials are irradiated by laser‐accelerated particles and by an in‐air plasma, both are techniques that have shown to heavily stress and damage materials used in laser‐matter interaction experiments. The authors observe that the chemical structure of the PEG reinforced materials, when irradiated by both techniques, stays unchanged. However, one can see that the PEG layer adds considerable longevity to the underlying materials, making it more robust against erosion and ablation occurring during its operation.