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We summarize our past five years of work on designing, building, and studying Sugilite, an interactive task learning agent that can learn new tasks and relevant associated concepts interactively from the user’s natural language instructions and demonstrations leveraging the graphical user interfaces (GUIs) of third-party mobile apps. Through its multi-modal and mixed-initiative approaches for Human-AI interaction, Sugilite made important contributions in improving the usability, applicability, generalizability, flexibility, robustness, and shareability of interactive task learning agents. Sugilite also represents a new human-AI interaction paradigm for interactive task learning, where it uses existing app GUIs as a medium for users to communicate their intents with an AI agent instead of the interfaces for users to interact with the underlying computing services. In this chapter, we describe the Sugilite system, explain the design and implementation of its key features, and show a prototype in the form of a conversational assistant on Android.