The roles of self-regulation and structuration in mobile learning are poorly understood. This study therefore examines these aspects in relation to the design and use of mobile technology in an online language learning setting. The online Self-Regulated Learning (SRL) instrument was adopted to measure students’ perceived level of self-regulation. Structuration Theory (ST) was applied as the theoretical lens for understanding students’ technology-mediated learning practices. The results show that several factors defining learners’ level of self-regulation were correlated with their mode of structuration. The analysis indicates that students’ SRL characteristics are strongly correlated with their structures regarding their technologies-in-practice and their practical assumptions about effectiveness in learning. An implication for practice is that students’ SRL dimensions need to be taken into account when designing educational software for mobile technology. For research, this study has demonstrated the explanatory power of ST and how students’ structures are related to their SRL characteristics.