Self-assembled Bi2Te3 one-dimensional nanorod bundles have been fabricated by a low-cost and facile solvothermal method with ethylene diamine tetraacetic acid as an additive. The phase structures and morphologies of the samples were characterized by X-ray diffraction, scanning electron microscopy, Fourier-transform infrared spectrometry, and transmission electron microscope measurements. The growth mechanisms have been proposed based on the experimental results. The full thermoelectric properties of the nanorod bundles have been characterized and show a large improvement in the thermal conductivity attributed to phonon scattering of the nanostructures and then enhance the thermoelectric figure of merit. This work is promising for the realization of new types of highly efficient thermoelectric semiconductors by this method.