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Based on the microbumps of graphene nanosheets and the nanostructure of carbon nanotubes (CNTs), novel graphene/CNTs composite films with hierarchical micro-and nanoscale surface roughness were successfully fabricated by simply spraying the mixed acetone dispersion of graphene nanosheets and CNTs onto stainless steel substrates. The as-prepared composite films exhibited controlled surface hydrophobic, adhesive and electrowetting properties via altering the film surface structure and surface energy. Among them the composite film with a 1 : 5 mass ratio of graphene to CNTs showed high hydrophobicity and conductivity, low water adhesion and contact angle sensitivity to the external electric field, which would help to resolve the surface electrostatic problems and unstable hydrophobicity under applied potential that exist in many conventional insulating hydrophobic materials, and could be useful in some application fields.

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