Ternary PbBi2S4 is a potential thermoelectric material with intrinsically low lattice thermal conductivity, but the low electrical transport properties limit its thermoelectric properties. In this work, high-quality ternary PbBi2S4 crystal ingots were prepared by the Bridgman method. By reducing the grain boundary density to reduce the carrier transport barrier, the electrical transport properties greatly improved. By optimizing the growth conditions, ternary PbBi2S4 crystal ingots of different qualities were obtained. The optimal weighted mobility increases from 15 cm2 /(V·s) in the polycrystal to 56 cm2 /(V·s), and the maximum electrical conductivity and power factor of the ternary PbBi2S4 crystal ingot reach 1 049 S/cm and 4.6 μW/(cm·K2 ), respectively. Compared with those of the polycrystalline PbBi2S4 sample, the increases are 850% and ~64%, respectively. Finally, the maximum ZT value in the PbBi2S4 crystal ingot reaches 0.61 at 773 K. The results show that the solidification growth of high-quality crystal ingots can significantly optimize the full-temperature thermoelectric properties of the ternary PbBi2S4 compound.