Single-phased β-Zn4Sb3 and β-Zn4Sb3/ Zn1-δAlδO composites with different amounts of Zn1-δAlδO (AZO) are prepared by the combination of vacuum melting and spark plasma sintering (SPS). Thermoelectric properties of the materials are investigated in a temperature range from 300 K to 673 K. As a result, the electrical conductivity of each sample increases while the Seebeck coefficient and the thermal conductivity decrease with the increase of AZO. The maximum ZT value of the composite reaches 1.16 at 673 K when the amount of AZO is 0.2 wt%, which is higher than that for the single-phased β-Zn4Sb3 (1.03).