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In this chapter, we present the Mobile Technology Capacity Building (MTCB) Framework, designed to enhance students’ appropriate use of personal mobile devices (PMDs) in workplace learning (WPL). WPL is a concept that denotes students’ learning that occurs in workplaces as part of their university curriculum. The workplace provides an environment for university students where learning and working and theory and practice are entwined. As such, WPL is an in-between or hybrid space where traditional roles, identities, and cultures are fluid and in transition. In the 21st century, where PMDs are more and more intricately interwoven into everyday personal, educational, and professional practices, learning with mobile technology offers new opportunities and possibilities to enhance WPL. The MTCB Framework for WPL focuses on cultivating agency and thoughtful consideration for practice contexts. Its development is underpinned by three sets of theoretical ideas: agentic learning, activity-centered learning design, and the entanglement of technology, learning, and work. Its design also draws on empirical data derived from surveys and interviews from 214 participants, including students, academics, and workplace educators that highlight the importance of considering workplace cultures. We conclude that the MTCB Framework addresses an urgent need for all stakeholders in WPL to build their capacity to use mobile technology effectively to contribute to enhancing WPL. Without a shared understanding of the role of mobile technology in WPL, it will remain difficult for students to make the most of the learning opportunities afforded by the use of PMDs in WPL.