In this study, zinc indium tin oxide thin-film transistors (ZITO TFTs) were fabricated by the radio frequency (RF) sputtering deposition method. Adding indium cations to ZnO by co-sputtering allows the development of ZITO TFTs with improved performance. Material characterization revealed that ZITO TFTs have a threshold voltage of 0.9 V, a subthreshold swing of 0.294 V/decade, a field-effect mobility of 5.32 cm2/Vs, and an on-off ratio of 4.7 × 105. Furthermore, an investigation of the photosensitivity of the fabricated devices was conducted by an illumination test. The responsivity of ZITO TFTs was 26 mA/W, with 330-nm illumination and a gate bias of -1 V. The UV-to-visible rejection ratio for ZITO TFTs was 2706. ZITO TFTs were observed to have greater UV light sensitivity than that of ZnO TFTs. We believe that these results suggest a significant step toward achieving high photosensitivity. In addition, the ZITO semiconductor system could be a promising candidate for use in high performance transparent TFTs, as well as further sensing applications.