We have demonstrated a new synthesis of twist-shaped nanocoiled and herringbone-type double micro-coiled carbon fibers via catalytic chemical vapor deposition of acetylene over NiCuMgAl-layered double hydroxides. The materials were characterized by power X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and N-2 adsorption-desorption experiments. For the first time, the use of electrodes modified with platinum particles supported on as-grown helical carbon fibers was studied for electrocatalytic oxidation of methanol. Especially, the electrode supported on herringbone-type double micro-coiled carbon fiber showed much larger Pt active surface area than that supported on commercial carbon black. Furthermore, such electrocatalyst has exhibited about fourfold enhancement of activity and excellent anti-poisoning ability, which is believed to be attributed to the combined beneficial effects of novel microstructure and special composition of as-grown helical carbon fibers. (C) 2010 Elsevier Ltd. All rights reserved.