Problematic smartphone use negatively affects physical and mental health. Despite the wide range of prior research, existing persuasive techniques are not flexible enough to provide dynamic persuasion content based on users' physical contexts and mental states. We first conduct a Wizard-of-Oz study (N=12) and an interview study (N=10) to summarize the mental states behind problematic smartphone use: boredom, stress, and inertia. This informs our design of four persuasion strategies: understanding, comforting, evoking, and scaffolding habits. We leverage large language models (LLMs) to enable the automatic and dynamic generation of effective persuasion content. We develop MindShift, a novel LLM-powered problematic smartphone use intervention technique. MindShift takes users' in-the-moment physical contexts, mental states, app usage behaviors, users' goals & habits as input, and generates high-quality and flexible persuasive content with appropriate persuasion strategies. We conduct a 5-week field experiment (N=25) to compare MindShift with baseline techniques. The results show that MindShift significantly improves intervention acceptance rates by 17.8-22.5% and reduces smartphone use frequency by 12.1-14.4%. Moreover, users have a significant drop in smartphone addiction scale scores and a rise in self-efficacy. Our study sheds light on the potential of leveraging LLMs for context-aware persuasion in other behavior change domains.
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