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Carbon nanofibers can be produced from graphene, graphite powder and carbon nanotubes by nozzle-less electrospinning and following stabilization and carbonization process. The prepared carbon nanofibers were used for the adsorption of Cr(VI) ions, and the adsorption performance of Cr(VI) ions under different test conditions were studied. It was 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. This features contribute to increasing the adsorption performance of adsorbent materials on Cr(VI) ions. Their adsorption capacity for Cr(VI) ions can reach 52.8 mg/g at pH=3, 25℃. Moreover, the adsorption capacity can remain about 60% of the initial adsorption capacity after five cycles. Therefore, the carbon nanotubes-based nanofibers exhibit the best adsorption performance. Hence, carbon nanotubes-based nanofibers have a promising in practice for applications in heavy metal ions adsorption due to their high specific surface area, high porosity, excellent surface chemistry and good adsorption performance.