A three-dimensional (3D) composite film containing copper nanostructures and carbon nanotubes (3DC/CNT composite film) was fabricated by one-step electrodeposition. The 3DC/CNT composite film was formed under galvanostatic conditions using a copper sulfate bath containing CNTs and polyacrylic acid which acts as both a 3DC-forming and a CNT-dispersing agent. The composite film consists of thin copper sheets with thicknesses of ca. 70-80 nm and CNTs, with large interior spaces between sheets. The CNTs were homogeneously distributed inside the composite film and were fixed by the copper sheets where CNTs pierce the copper sheets. The CNT content in the composite films increased with the CNT concentration of the plating bath. The 3DC film without CNTs did not maintain its 3D spaces when the film thickness was increased due to insufficient structural strength, whereas the 3DC/CNT composite film maintained the 3D spaces despite an increase in film thickness, which suggests that the CNTs reinforce the film to maintain the 3D spaces. Three-dimensional (3D) nanostructured metal architectures typically exhibit large specific surface areas and high electrical conductivity; therefore, their application as electrodes in functional devices such as supercapacitors, 1 fuel cells 2 and batteries 3 have been widely researched. For these potential applications, the use of 3D copper nanostructured architectures 4-8 is most attractive. However, although 3D copper nanostructured architectures are very effective to improve electrode functions, their manufacture requires many steps and is therefore complex. Our group has previously developed a very straightforward method for the fabrication of 3D copper nanostructured architectures by electrodeposition, in which an organic additive is simply added to an electrodeposition bath.9 This process for the preparation of 3D copper nanostructured architecture films by onestep electrodeposition (the resulting products henceforth being designated as 3DC1 film) is expected to be used as a practical method for the fabrication of various components, such as current collectors for tin-based lithium-ion battery anodes.10 However, the 3DC1 film consists of very thin (30-50 nm) copper sheets; therefore, its structural strength is low, which results in deformation of the 3D structure when a slight physical force is applied.In contrast, carbon nanotubes (CNTs) 11,12 have excellent mechanical characteristics, 13-15 such as high tensile strength and high elastic modulus, in addition to high thermal [16][17][18] and electrical conductivity. 19,20 Research into CNT composites such as metal/CNT composites has thus been actively pursued.21,22 A 3D-copper nanostructured architecture containing CNTs (3DC/CNT composite) is thus considered to be an attractive copper-based 3D composite material that would have sufficient structural strength due to the reinforcement effect of the CNTs. If a 3DC/CNT composite could be fabricated by a simple method, then the 3DC/CNT composite materials would be expected to be used for ...