Free-standing and conductive aligned carbon nanotubes (ACNT) were described that act as an efficient, robust, high surface area electrocatalysts when coated with Pt nanoparticles. Pt nanoparticles were electrodeposited on the ACNT array by cyclic voltammetry from 0.01 M H2PtCl6/0.5 M NaNO3/H2O. The EASSA of electrodeposited Pt nanoparticles on the PVDF/ACNT array is found to be 143∓14.3 m2g -1. Cyclic voltammetry in 1 M CH3OH/1 M H 2SO4/Pt/PVDF electrode display an enhanced performance and a more negative starting potential for methanol oxidation than an ITO electrode. The atom efficiency and robustness of the nano-Pt-ACNT/Pt/PVDF arrays is confirmed in potentiostatic studies of hydrogen reduction catalysis.