Recently, Te1-xSex films have shown significant potential for infrared detection. However, the conventional deposition process of Te1-xSex films typically requires a cooled substrate, which results in the formation of poorly crystallized materials. Achieving controlled synthesis of large-area Te1-xSex films remains a major challenge. Herein, two-inch Te1-xSex films is successfully prepared using a low-pressure chemical vapor deposition technique based on a selenium phase transition-induced strategy. The chemical compositions of Te1-xSex (x ranging from 0 to 1) films can be precisely controlled by adjusting the molar ratio of Te and Se powders. The phase change of amorphous Se at elevated temperatures generates additional dangling bonds on its surface, which facilitates the incorporation of Te atoms into Se chains forming Te1-xSex alloys. COMSOL simulations reveal that maintaining uniform concentration and temperature during the growth process is essential for the formation of Te1-xSex films. Importantly, the Te0.4Se0.6 film detector realizes high-performance near-infrared single-pixel imaging with a resolution of 128 × 128 pixels. This work has fabricated wafer-scale Te1-xSex alloy thin films, which exhibit excellent properties, providing important experimental and theoretical support for exploring the applications in the fields of electronics, photonics, and optoelectronics.