Carbon nanotubes (CNTs) present a new material for the construction of electrodes. The large scale production of aligned carbon nanotube (ACNT) arrays was first reported by Dai and co-workers [1], providing an opportunity to develop highly ordered, high surface area electrodes with excellent electronic and mechanical properties. While the latter two attributes are realized in the vertical direction, there is a need to develop simple methods of making ACNT composites that are mechanically robust and with sufficient conductivity in the horizontal direction. Such interconnects would give rise to a practically useful electrode structure for use in applications such as energy storage [2], actuators [3] and sensors [4].Aligned CNT growth, while producing innovative structures, suffers from a lack of good electrical connectivity between the aligned tubes. Growth on conducting substrates which would provide this electrical connection has met with limited success; recently direct growth on metal alloys [5] has been reported. Depositing metals selectively on top of CNT arrays to achieve this electrical connection [6] is fraught with difficulties. To realize the potential of these arrays in applications such as flexible displays, their removal from the substrate used for growth is necessary. Invariably, removal of the CNT array from surfaces results in damage, including breakdown of any metal coated on top to achieve an electrical connection. To address this issue of lack of robust electrical connection between nanotubes in an array, we present here an approach for preparing a nanostructured ACNT/conducting polymer composite. Organic conducting polymers have proven to be useful in the development of polymer-based composites [7][8][9]. In the novel nanostructure created here, the CNT's are held together by a conducting polymer composite layer. The nanotubes remain vertically oriented and protrude from the conducting polymer layer (90 % of the tube length is exposed). The electrochemistry of the nanostructured electrodes produced and their use as the anode material in Li-ion batteries are presented.In this study, poly(3,4-ethylenedioxythiophene) (PEDOT) was utilised as the conducting polymer due to the excellent electrochemical activity and electronic conductivity attainable with this material. A thin PEDOT film was deposited onto the ACNT array by chemical vapour phase polymerization (CVP). The procedure used to form the nanostructured electrode from a quartz plate is summarized in Scheme 1. Aligned multi-wall carbon nanotubes were produced by pyrolysis of iron(II) phthalocyanine as described by Dai [1,10]. Following production of the aligned CNTs on a quartz plate, a thin PEDOT film (100 nm thickness across the entire film) was deposited onto ACNT arrays by CVP using ferric p-toluenesulfonate (Fe(III) tosylate) as oxidant. The SEM image of this ACNT/PEDOT composite film (insert (a) in Scheme 1) indicates that the PEDOT deposited by VPP formed a continuous film on the top of the ACNT array. It was found that the PEDOT film ...