This article explores how to research the opportunities for emotional engagement that mobile technologies provide for the design and enactment of learning environments. In the context of mobile technologies that foster location-based linking, we make the case for the centrality of in situ real-time observational research on how emotional engagement unfolds and for the inclusion of bodily aspects of interaction. We propose that multimodal methods offer tools for observing emotion as a central facet of person-environment interaction and provide an example of these methods put into practice for a study of emotional engagement in mobile history learning. A multimodal analysis of video data from 16 pairs of 9- to 10-year-olds learning about the World War II history of their local Common is used to illustrate how students' emotional engagement was supported by their use of mobile devices through multimodal layering and linking of stimuli, the creation of digital artifacts, and changes in pace. These findings are significant for understanding the role of digital augmentation in fostering emotional engagement in history learning, informing how digital augmentation can be designed to effectively foster emotional engagement for learning, and providing insight into the benefits of multimodality as an analytical approach for examining emotion through bodily interaction.