The composites containing Ni nanoparticles and N-doped carbon nanotubes were prepared using Ni-Al layered double hydroxides (LDHs) with various Ni/Al atomic ratios (2 and 3) and acetonitrile via catalytic chemical vapor deposition at 600, 700 and 800 degrees C. Powder X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, thermogravimetric analysis and nitrogen sorption were employed to characterize their physicochemical properties. The electrochemical properties of the composites were evaluated by means of cyclic voltammetry in alkaline medium with the addition of methanol as a probe molecule. Application of different synthesis temperatures and Ni-Al LDHs with various Ni concentrations influenced the electrocatalytic performance of the composites for the methanol oxidation reaction as it affected the dispersion of Ni nanoparticles and electrode/electrolyte interfacial active area. The hybrid material prepared at the lowest temperature (600 degrees C) and derived from LDHs with a lower Ni/Al = 2 appeared to have the best electrochemical properties among the studied composites. (c) 2012 Elsevier Ltd. All rights reserved.