Bismuth sulfide (Bi2S3) polycrystalline bulks with a high relative density (>90%) were fabricated by combining mechanical alloying (MA) and spark plasma sintering (SPS). The microstructural and thermoelectric (TE) properties were investigated with a special emphasis on the influence of SPS temperature. The components (Bi/S ratio), grain size, and relative density of Bi2S3 bulk are sensitive to the SPS temperature, which all affect the electrical transport properties of samples. Elevating SPS temperature results in grain growth, densification, and spontaneous texturing, which benefit to enhance TE properties, whereas overheating leads to severe volatilization of both S and Bi and formation of porous microstructure. The highest figure of merit value reaches 0.22 at 573 K for the Bi2S3 sample obtained by applying SPS at 673 K for 5 min, which is the maximum value reported so far in bulk Bi2S3 system. The enhanced TE property of cheap and environmental friendly Bi2S3 material indicates a great promise in TE devices.