Currently, the picture book market for adult readers is on the rise, and the development of AR (Augmented Reality) technology has introduced new possibilities for its growth. This study aims to explore the factors that may influence the intention of adult readers to use AR picture books. We employed the Partial Least Squares Structural Equation Modeling (PLS-SEM) method for analysis. Through offline recruitment and experiential sessions, we collected and analyzed 332 valid questionnaires, constructing a structural equation model of adult AR picture book user behavior intentions. Functional experience, action experience, aesthetic experience, and emotional experience all have positive effect on the adults’ intention to use AR picture books. The path coefficients for these relationships are relatively close, at 0.275, 0.225, 0.176, and 0.267, respectively. Perceived interactivity has a positive effect on perceived playfulness, with the largest path coefficient among all relationship paths at 0.585. Furthermore, both perceived interactivity and perceived playfulness positively influence functional experience, action experience, aesthetic experience, and emotional experience. The path coefficients of perceived interactivity for these four experiences are 0.473, 0.388, 0.413, and 0.342, respectively, while those of perceived playfulness are 0.359, 0.368, 0.362, and 0.422, respectively. Based on these findings, the study offers recommendations for optimizing the design of AR picture books for adults, aiming to enhance their reading experience, meet their needs, and provide valuable guidance for the future development of this emerging industry.