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Abstract The broad implementation of thermoelectricity requires high‐performance and low‐cost materials. One possibility is employing surfactant‐free solution synthesis to produce nanopowders. We propose the strategy of functionalizing “naked” particles’ surface by inorganic molecules to control the nanostructure and, consequently, thermoelectric performance. In particular, we use bismuth thiolates to functionalize surfactant‐free SnTe particles’ surfaces. Upon thermal processing, bismuth thiolates decomposition renders SnTe‐Bi₂S₃nanocomposites with synergistic functions: 1) carrier concentration optimization by Bi doping; 2) Seebeck coefficient enhancement and bipolar effect suppression by energy filtering; and 3) lattice thermal conductivity reduction by small grain domains, grain boundaries and nanostructuration. Overall, the SnTe‐Bi₂S₃nanocomposites exhibit peakz Tup to 1.3 at 873 K and an averagez Tof ≈0.6 at 300–873 K, which is among the highest reported for solution‐processed SnTe.