Spark plasma sintering (SPS) is currently widely applied to existing alloys as a means of further enhancing the alloys' figure of merit. However, the determination of the optimal sintering condition is challenging in the SPS process. This report demonstrates a systematic way to independently optimize the Seebeck coefficient S and the ratio of electrical to thermal conductivity (σ /κ) and thus achieve the maximum figure of merit zT = S2 (σ /κ)T. Sb 2-x Inx Te3 (x = 0-0.2) were chosen as examples to validate the method. Although high sintering temperature and pressure are helpful in enhancing the compactness and electrical conductivity of pressed samples, the resultant deteriorated Seebeck coefficient and increasing thermal conductivity eventually offset the benefit. We found that the optimal sintering temperature coincides with temperatures at which the maximum Seebeck coefficient begins to degrade, whereas the optimal sintering pressure coincided with the pressure at which the σ /κ ratio reaches a maximum. Based on this principle, the optimized sintering conditions were determined, and the zT of Sb1.9 In0.1 Te3 is raised to 0.92 at 600 K, showing an approximately 84% enhancement. This work develops a facile strategy for selecting the optimal SPS sintering condition to further enhance the zT of bulk specimens.