This study investigated the effects of self-efficacy and self-regulation on student achievement in a context-aware learning environment. Particularly, an innovative global positioning system (GPS) sensor-based mobile learning system was used to facilitate English learning of different plants on campus. A total of 41 university students participated in the study, divided into high and low groups of self-efficacy and self-regulation. The findings showed that both self-regulation and self-efficacy were significant predictors of learning achievement in the mobile context-aware learning (MCL) context. Moreover, while the GPS-based MCL learning session had positive effects on learning achievement, no significant increase in self-regulation or self-efficacy was found in either the high or the low group, supposedly due to the short duration of the activity. The participants found the system easy to use and useful, but they also raised critical concerns that can inform future improvements. We hope this exploratory study can serve as a starting point from which more interactive, user-friendly GPS sensor-based learning systems will be generated and more areas of application will be further explored to foster self-regulated, self-motivated ubiquitous learning of mobile learners.