This study aimed to examine the factors that potentially impact the self-directed use of mobile English learning resources (MELR). The participants were 206 Chinese undergraduate EFL learners at Yangzhou University in Mainland China. Applying and modifying the Unified Theory of Acceptance and Use of Technology (UTAUT), this study involved six constructs, including students’ performance expectancy, effort expectancy, social influence, facilitating conditions, perceived playfulness, and behavioral intention to use MELR. The structural equation modeling (SEM) technique was adopted to analyze the data collected from the questionnaire. The findings showed that facilitating conditions acted as the most significant predictor of behavioral intention to adopt MELR, followed by effort expectancy, perceived playfulness, and performance expectancy. However, social influence did not have significant effects on students’ use of MELR. Pedagogical implications for teachers and students were also presented in the end.