The electrochemical properties of single-wall carbon nanotube (CNT) electrodes in the form of sheets or papers have been examined. Thermal annealing has produced significant changes in a range of properties of the material including increased hydrophobicity and elimination of electroactive surface functional groups and other impurities. As a result of these changes, the treated electrodes exhibit lower double-layer capacitance, absence of faradaic responses and associated pseudocapacitance, and a better frequency response. The basic electrochemical behavior of the CNT paper electrodes is not markedly affected by relatively large differences in electrolyte ion size, consistent with an average pore size of 9 nm. Increases in both CNT sheet thickness and surface area induce a slower electrode response in agreement with the porous nature of the electrode matrix. (C) 2003 The Electrochemical Society.