As a potential thermoelectric (TE) material, the high lattice thermal conductivity and relatively low weighted mobility severely limit TE property optimization of InSb binary compound. In this paper, we substituted In of InSb with Ga and systematically investigated the effect of Ga alloying on the Seebeck coefficient, electrical conductivity and lattice thermal conductivity of InSb between 300 K and 770 K. We found that Ga alloying simultaneously reduced the lattice thermal conductivity and optimized the weighted mobility of InSb. The lattice thermal conductivity has been analyzed using Abeles model to gain more insight on the roles of Ga in In1-xGaxSb (x = 0, 0.1, 0.15, 0.2) solid solution. The synergetic effect of Ga alloying on the electron and phonon transport leads to a marked enhancement in TE potential of InSb. The dimensionless figures of merit of InSb and In0.8Ga0.2Sb reach, respectively, 0.54 and 0.52 at 770 K.