Human memory is context-dependent, meaning that our internal and external environments becomes bound with memories that we form, thus affecting how well we learn and remember. This dissertation research used virtual reality (VR) to exploit this quirk to improve learning and retention. We found that learning two similar languages each in a distinct VR helped participants retain 92% of what they had learnt one-week later---but only if they had experienced VR as "real" environments. Moreover, using functional neuroimaging, this work identified brain patterns behind this effect, and provide novel and concrete evidence of contextually-supported memory recall and retention. Theoretical and technical implications of this work is discussed in terms of furtherance of neuroimaging and memory research, as well as possible clinical application and educational interventions. Additional discussions of the current state of the arts was also included for VR applications in neuroimaging, and applications of neuroimaging techniques in memory research.