We investigated the thermoelectric properties of the InSe, InSe/In4Se3 composite, and SrTiO3 (STO) nano-particles dispersed InSe/In4Se3 bulk composites. The electrical conductivity of the InSe/In4Se3 composite with self-assembled phase separation is significantly increased compared with those of InSe and In4Se3–δ implying the enhancement of surface conductivity between grain boundaries. The thermal conductivity of InSe/In4Se3 composite is decreased compared to those of InSe. When the STO nano-particle dispersion was employed in the InSe/In4Se3 composite, a coherent interface was observed between nano-particle precipitates and the InSe bulk matrix with a reduction of the thermal conductivity.