Highly porous carbons have been successfully synthesized by chemical activation of polythiophene with KOH. The activation process was performed under relatively mild activation conditions, i. e., a KOH/polymer weight ratio of 2 and reaction temperatures in the 600-850 degrees C range. The porous carbons thus obtained possess very large surface areas, up to 3000 m(2)/g, and pore volumes of up to 1.75 cm(3)/g. The pore size distribution of these carbons can be tuned via modification of the activation temperature. Thus, by increasing the activation temperature from 600 to 850 degrees C, the nature of the carbons changes gradually from microporous to micro-mesoporous (with small mesopores of up to 2.5 nm). The polythiophene-derived activated carbons are sulfur-doped with sulfur contents in the 3-12 wt% range. The sulfur content decreases at higher activation temperature. The hydrogen storage capacity of these activated carbons, at cryogenic temperature and 20 bar, is up to 5.71 wt% with an estimated maximum hydrogen uptake of 6.64 wt%. Their ease of preparation and high uptake makes the polythiophene-derived carbons attractive hydrogen storage materials. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.