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In this Article, bulk-quantity one-dimensional polyaniline (1D PANI) nanowire/tubes with rough surface were prepared by a simple chemical oxidation method. This kind of PANI nanostructure can not only remove Cr(VI) rapidly and effectively in one step from aqueous solution by reducing Cr(VI) to Cr(III) as well as adsorbing the reduced Cr(III) simultaneously, but also be easily regenerated for reuse. During the removal of Cr(VI) process, the as-synthesized PANI was oxidized from emeraldine salt to pernigraniline, and pernigraniline could be reconverted into emeraldine salt by acid treatment. In addition, the morphology of the PANI was not changed after used for Cr(VI) removal. This study not only provides a facile way to fabricate bulk-quantity 1D PANI nanostructure, but also shows a reproducible material for removal of toxic Cr(VI) from wastewater.