Bis(ethylenedithio)tetrathiafulvalene(BEDT-TTF; Scheme 1) based charge-transfer salts have been intensively studied since the initial synthesis of neutral BEDT-TTF molecules.[1] These salts exhibit many interesting solid-state physical properties such as superconductivity, [2][3][4][5] conductor-toinsulator transitions, [6][7][8] antiferromagnetism, [5,7,9] or ferromagnetism.[4] The basic structure of BEDT-TTF-based salt crystals is composed of two alternating layers: a BEDT-TTF cation layer and an anion layer. The anions can be varied in terms of size, charge, and structure, giving rise to the properties mentioned above. However, most of these physical properties were investigated on macroscopic single-crystalline samples to explore the anisotropic characteristics of the properties. To advance these materials for potential applications, such as interfacial materials for organic molecules and inorganic substrates, or to probe the size effect on the superconductivity of these materials, quasi-1D BEDT-TTF-based systems, including nanotubes and nanowires, with controlled size and morphology are important. To our best knowledge, there have been no reports in the literature on the fabrication of BEDT-TTF-based charge-transfer salt nanotubes. In addition, although the electrical characteristics of single crystals and films of BEDT-TTF-based charge-transfer salts have been well studied [10][11][12][13][14][15] the electrical conductivity of one dimensional materials has rarely been investigated.Porous anodic aluminum oxide (AAO) membranes have a well-defined close-packed array of columnar hexagonal cells, each containing a central pore with different shapes normal to the surface.[16] They are ideal host systems for the fabrication of large-area nanostructures (nanotubes and nanowires). Moreover, the length and diameter of these nanostructures can be readily tailored by changing the thickness and pore diameter of the AAO templates. A variety of metals, [17][18][19][20] semiconductors, [21][22][23] and hybrid materials [24,25] have been synthesized using various methods based on AAO templates, which were pioneered by Martin and co-workers. [26,27] Various other 1D inorganic materials have been synthesized and well studied, [28][29][30][31][32][33] while only a few reports focus on organic materials [34][35][36] and devices based on them. [37,38] Herein, we describe a simple route to the fabrication of large-area BEDT-TTF-and tris(oxalate)iron-based chargetransfer salt nanotubes from an electrochemical process on an AAO anode. The morphology of these nanotubes was readily tuned by varying the pore shapes and apertures of the AAO templates or by changing the electrocrystallization time. The fabrication procedure can be regarded as a model for fabricating nanotubes of other interesting charge-transfer salts. The current-voltage (I-V) characteristics and temperature-dependent electrical conductivity of synthesized nanotube arrays were studied by constructing an electrical circuit with nanotube arrays, and the I-V characterist...