The exploration of new synthesis methods is important for the improvement of the thermoelectric property of a material for the different mechanisms of microstructure fabrication, surface activity modulation, and particle refinement. Herein, we prepared p-Bi2Te3 bulk materials by a simple synthesis method of the plasma-assisted ball milling, which yielded finer nanopowders, higher texture of in-plane direction, and higher efficiency compared to the traditional ball milling, favoring the simultaneous improvement of electrical and thermal properties. When combined with the Te liquid sintering, nano-/microscale hierarchical pores were fabricated and the carrier mobility was also increased, which together resulted in the low lattice thermal conductivity of 0.52 W·m–1·K–1 and the high power factor of 43.4 μW·cm–1·K–2 at 300 K, as well as the ranking ahead zT of 1.4@375 K. Thus, this work demonstrated the advantages of plasma-assisted ball milling in highly efficient synthesis of p-type Bi2Te3 with promising thermoelectric performance, which can also be utilized to prepare other thermoelectric materials.

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