The effects of high-temperature solid-state reactions on the microstructures, optical properties, photoactivity, and low-concentration NO 2 gas-sensing sensitivity of ZnO-SnO 2 core-shell nanorods were investigated. In this study, the ZnO-SnO 2 core-shell nanorods were synthesized through a combination of the hydrothermal method and vacuum sputtering. According to X-ray diffraction and transmission electron microscopy analyses, high-temperature solid-state reactions between the SnO 2 shell and ZnO core materials at 900 C engendered an ultrathin SnO 2 shell layer for transforming into the ternary Zn 2 SnO 4 (ZTO) phase. Moreover, surface roughening was involved in the high-temperature solidstate reactions, as determined from electron microscopy images. Comparatively, the ZnO-ZTO nanorods have a higher oxygen vacancy density near the nanostructure surfaces than do the ZnO-SnO 2 nanorods.The photodegradation of rhodamine B dyes under simulated solar light irradiation in presence of the ZnO-SnO 2 and ZnO-ZTO nanorods revealed that the ZnO-ZTO nanorods have a higher photocatalytic activity than do the ZnO-SnO 2 nanorods. Furthermore, the ZnO-ZTO nanorods exhibited higher gassensing sensitivity than did the ZnO-SnO 2 nanorods on exposure to low-concentration NO 2 gases. The substantial differences in the microstructure and optical properties between the ZnO-SnO 2 and ZnO-ZTO nanorods accounted for the photocatalytic activity and NO 2 gas-sensing results obtained in this study.