Zero Valent Iron nanoparticles (nZVI) were synthesized and immobilized on electrospun carbon nanofibers (ECNFs) surface in a controllable manner through redox reaction. The novel nanomaterial, ECNFs-supported nZVI (nZVI@ECNFs), were evaluated for Cr(VI) ions removal from water for the first time. nZVI@ECNFs outperformed stand-alone nZVI as well as state-ofthe- art nZVI research for Cr(VI) remediation in water. nZVI@ECNFs with 0.4 g/L nZVI loading could remove 100% Cr(VI) from 50 mg/L Cr(VI) aqueous solution in as little as 5 min at pH = 4. This is enabled by coupling nanofibrous form ECNFs with dispersed distribution of individual and/or cluster nZVI on surface of ECNFs. It is envisioned that nZVI@CNFs is going to serve as a novel supported nZVI nanomaterial for super-fast heavy metal remediation in ground water and waste water treatment with adjustable high capacity as well as straightforward and energysaving heavy metal recovery.