Computational thinking (CT) currently has been mainly explored using programming robots and conducted in K12 education. In early childhood education, arts have a significant place in children’s learning, expression and cognitive development. Specifically, creating pop-up storybooks is a child-friendly activity. Our study aimed to explore the combination of CT and art, and to develop talented children’s CT abilities through a multimodal literacies educational approach, which referred to using different skills (i.e., writing, drawing, making, and storytelling) in the art activity. A total of 12 talented children were selected to participate in a pop-up storybook production workshop using a convenience sampling method. We adopted an observation method to capture talented children’s CT behaviors, generating a total of 180 min of activity videos and collecting fieldnotes and the children’s worksheets and artworks for the data analysis. Based on a content analysis, we found that talented children enhanced their CT development in multiple modes and practiced seven CT skills. In conclusion, our study emphasizes the importance of art in children’s education and provides new insights for subsequent research on children’s CT education.