A growing number of studies are focusing on the effect of teachers' knowledge on their behavioral intention to use technology in teaching. This study aims to explore the influence of teachers' technological pedagogical content knowledge (TPACK) on their behavioral intention to use technology by including their technology self-efficacy and attitude toward use in a chain mediation model. Based on a thorough literature review, this study establishes a theoretical model. Then, data are collected from 314 in-service teachers in primary and secondary schools in two provinces in China and analyzed using structural equation modeling and effect analysis. Results show that (1) the teachers' technology self-efficacy and attitude toward technology play a crucial independent mediating role in the influence of TPACK on their behavioral intention to use technology, and (2) the teachers' technology self-efficacy and attitude toward use have a chain mediating effect on the influence of their TPACK on their behavioral intention to use technology. On the basis of the results, this study presents some implications to effectively understand how teachers' behavioral intention to use technology in teaching can be improved.