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Mobile technologies are now ubiquitous in Low- and Middle-Income Countries (LMICs). Education in LMICs is among the latest disciplines set out to explore how mobile technologies’ particular affordances can be used to support programme interventions and practice. However, neither the effectiveness of mobile learning programmes, nor the causal mechanisms and contexts through which teaching and learning with mobile technologies is assumed to support education and development in LMICs, have been systematically reviewed and conceptualised. Notwithstanding, learning and teaching with mobiles is regularly attributed as having the potential to change and improve education in LMICs. This thesis assesses the effectiveness and underlying theory of change of mobile learning programmes in LMICs through a mixed-methods systematic review, including meta-analysis and thematic synthesis. Building on the findings of the systematic review, it presents the Capability Approach as a theoretical lens through which to conceptualise the effects of mobile technologies on education and development in LMICs. Reviewing the evidence-base and theory of change of the application of mobile technologies as an educational tool in LMICs, I find little evidence to support claims to mobile learning’s potential to support development outcomes. These systematic review findings are then expanded in a qualitative case study of a mobile learning project in rural South Africa exploring teachers’ use of mobile technologies from the perspective of the Capability Approach. The case study finds that teachers’ use of mobile technologies can best be understood as an expansion in four dimensions of capabilities: informational, educational, societal, and economic capabilities, which taken together can enhance teachers’ well-being and human development. I use the combined case study and systematic review findings to reposition mobile learning’s role in international development. I argue that conceptualising mobile learning for development through the Capability Approach supports a focus on an endogenous transformation of education in LMICs anchored in the primary objective of enhancing the capabilities and agency of actors in the education system. In the absence of evidence supporting mobile learning’s impact on development outcomes, a focus on the role of mobile technologies to expand teachers’ and learners’ valued functionings and capabilities is presented as an alternative conception of the links between mobile technologies, their use for educational purposes in LMICs, and development outcomes.