Moodle is widely used in higher education institutions in this digital age. With the growing popularity of Moodle use in education, this study aimed to research on the factors that influence student users’ intentions to adopt Moodle for learning purposes in Macau. A total of 564 students from nine departments at the University of Macau responded to a survey in which ten constructs from a framework that integrated the Diffusion of Innovation Theory and Technology Acceptance Model, were measured. The results of this study showed that the research model had a good fit. Two variables—usefulness and ease of use—had significantly influenced Macau students’ attitudes towards Moodle use. Other variables such as usefulness, attitude, and perceived behavioral control were found to be important determinants of students’ behavioral intentions. Furthermore, usefulness was significantly associated with ease of use, output quality, trialability, as well as subjective norm. Students’ perceptions on the ease of use was significantly influenced by technology complexity and trialability. On the whole, the proposed research model had explained 66% of the variance of Macau university students’ behavioral intentions to use Moodle. This study contributed to deepening our understanding of technology acceptance theories by contextualizing the current study within the Macau higher education.