We prepared nanostructured carbon fiber surfaces using chemical vapor deposition in which Ni nanoparticles were used as carbon nanostructure growth catalysts. The surface of the nanostructured carbon fiber was covered by a thin polydimethylsiloxane film. This surface showed superhydrophobic behavior with a water contact angle close to 170 °C, and its superhydrophobicity was sustained in a wide pH range (1-13).