AbstractSemiconducting â-Zn4Sb3and ZrNiSn-based half-heusler compound thin films were prepared by co-evaporation for the application of thermoelectric (TE) materials. High-purity solid zinc and antimony were evaporated by electron beam to grow the â-Zn4Sb3thin film while high-purity zirconium powder and nickel tin powders were evaporated by electron beam to grow the ZrNiSn-based half-heusler compound thin film. Rutherford backscattering spectrometry (RBS) was used to analyze the composition of the thin films. The grown thin films were subjected to 5 MeV Si ions bombardments for generation of nanostructures in the films. We measured the thermal conductivity, Seebeck coefficient, and electrical conductivity of these two systems before and after 5 MeV Si ions beam bombardments. The two material systems have been identified as promising TE materials for the application of thermal-to-electrical energy conversion, but the efficiency still limits their applications. The electronic energy deposited due to ionization in the track of MeV ion beam can cause localized crystallization. The nanostructures produced by MeV ion beam can cause significant change in both the electrical and the thermal conductivity of thin films, thereby improving the efficiency. We used the 3ù-method measurement system to measure the cross-plane thermal conductivity ,the Van der Pauw measurement system to measure the cross-plane electrical conductivity, and the Seebeck-coefficient measurement system to measure the cross-plane Seebeck coefficient. The thermoelectric figures of merit of the two material systems were then derived by calculations using the measurement results. The MeV ion-beam bombardment was found to decrease the thermal conductivity of thin films and increase the efficiency of thermal-to-electrical energy conversion.