Carbon nanofibers were produced using graphene, graphite powder and carbon nanotubes as carbon sources by nozzle-less electrospinning followed by stabilization and carbonization process. The adsorption performance of carbon nanofibers to Cr(VI) ions under different test conditions was studied. It is found that carbon nanotubes-based nanofibers exhibit a large surface roughness, the best degree of graphitization, more ordered crystal structure, and the largest specific surface areas, which help to increase the adsorption performance of adsorbent materials to Cr(VI) ions. The adsorption capacity to Cr(VI) ions can reach 52.8 mg/g at pH=3, and T=25 degrees C. Moreover, the adsorption capacity can be about 60% of the initial adsorption capacity after five cycles.