N-type (Bi2Te3)0.93(Bi2Se3)0.07 thermoelectric materials doped with various content of TeI4 (0, 0.05, 0.08, 0.10, 0.13, and 0.15wt%) have been fabricated through the combination of zone melting and spark plasma Sintering. Electrical conductivity (σ), Seebeck coefficient (α) and thermal conductivity (κ) were measured in the temperature range of 300—500K. The influence of the variation of TeI4 content on thermoelectric properties was studied. The increase of TeI4 content caused an increase of carrier concentration and thus resulted in an increase of σ and a decrease of α, and the lattice thermal conductivity was decreased by the increase of phonon scattering resulting from heterogeneous ion (I) scattering and carrier scattering. The maximum figure of merit ZT (ZT=α2σT/κ) of the sintered materials in the direction perpendicular to the pressing direction showed a value of 0.92 for the sample containing 0.08wt% TeI4. In addition, the bending strength of the sintered materials was improved to about 80MPa from about 10MPa of the zone-melted ingot, which is of advantage to the fabrication process and the improvement of the reliability for thermoelectric modules.