This paper’s focus is on the development of research methodologies to investigate learning in higher education. These methodologies have made use of Social Mobile Devices (SMD) for data collection, a relativity new concept in qualitative research. The paper provides examples of practice linked with discussions from the Learning Without Frontiers Conference 2011 (LWF 2011) around the constraints, affordances, and ethical issues inherent in the use of SMDs for research. While the researchers used Apple iPhones and Apple iPads, this should not limit the applicability of the paper to other devices. It is hoped that this paper will aid the development of these tools for research purposes in the future through wider discussion, use, and dissemination. Technological development of SMDs continues unabated, hence developing methodologies around their use is an important task that will enable researchers to take advantage of the future applications they provide, whilst being aware of their impact upon the research process.