This paper investigated the factors affecting the behavioral intention (BI) and usage behavior (UB) of 548 Chinese college students in massive open online courses (MOOCs). We extended the unified theory of acceptance and use of technology model by incorporating self‐regulated learning (SRL) management, perceived pleasure (PP), and perceived cost constructs. This study also analyzed the moderating role of individual differences in gender, grade, major, and experience in MOOCs. Data were collected through both offline surveys across 10 universities and an online survey platform. Results from structural equation modeling and multi‐linear regression analyses revealed that students' BI was significantly and positively influenced by six factors: performance expectancy, effort expectancy, facilitating conditions (FC), social influence, SRL management (SM), and PP. Furthermore, we found that UB was predicted by BI, FC, and SM. Moreover, BI played a mediating role in the relationship between the two determining variables (i.e., FC and SM) and UB. Differences in MOOC experience level had a moderation effect. The study provided implications for various stakeholders regarding designing MOOC platforms, structures, and teaching activities.