The effect of dimensionality and nanostructure on thermoelectric properties in Bi2Te3-based nanomaterials is summarized. Stoichiometric, single-crystalline Bi2Te3 nanowires were prepared by potential-pulsed electrochemical deposition in a nanostructured Al2O3 matrix, yielding transport in the basal plane. Polycrystalline, textured Sb2Te3 and Bi2Te3 thin films were grown at room temperature using molecular beam epitaxy and subsequently annealed at 250A degrees C. Sb2Te3 films revealed low charge carrier density of 2.6 x 10(19) cm(-3), large thermopower of 130 V K-1, and large charge carrier mobility of 402 cm(2) V-1 s(-1). Bi-2(Te0.91Se0.09)(3) and (Bi0.26Sb0.74)(2)Te-3 nanostructured bulk samples were prepared from as-cast materials by ball milling and subsequent spark plasma sintering, yielding grain sizes of 50 nm and thermal diffusivities reduced by 60\%. Structure, chemical composition, as well as electronic and phononic excitations were investigated by x-ray and electron diffraction, nuclear resonance scattering, and analytical energy-filtered transmission electron microscopy. calculations yielded point defect energies, excitation spectra, and band structure. Mechanisms limiting the thermoelectric figure of merit for Bi2Te3 nanomaterials are discussed.