TAGS-90 compound powder was directly prepared from the elements by high-energy ball milling (HEBM) and subsequently consolidated by a spark plasma sintering (SPS). Effect of milling time on the microstructure and thermoelectric properties of the samples were investigated. The particle size of fabricated powders were decreased with increasing milling time, finally fine particles with ~1μm size was obtained at 90 min. The SPS samples exhibited higher relative densities (>99%) with fine grain size. X-ray diffraction analysis (XRD) and energy dispersion analysis (EDS) results revealed that all the samples were single phase of GeTe with exact composition. The electrical conductivity of samples were decreased with milling time, whereas Seebeck coefficient increased over the temperature range of RT~450°C. The highest power factor was 1.12×10−3W/mK2 obtained for the sample with 90 min milling at 450°C.