Books and paper prints are the most common learning medium we used to have. However, content knowledge represented in books and paper prints is static, which limits the manifestation of complex and abstract concepts. Integrating smartphone with books makes it possible to incorporate varieties of digital materials fetched from the Internet to complement the content of books and paper prints and enrich the learning activities. Collaborative learning has been recognized as an effective instructional strategy. Individual learners learn through continuous conversation with group peers for knowledge sharing and knowledge construction. However, it has also been reported that the lack of proper procedural facilitation may undermine the learning performance of collaboration. To ensure that every learner in a group can best contribute to peer collaboration, a procedural scaffold was designed and implemented. The scaffolded procedure consists of four stages in peer collaboration, including individual learning, individual problem solving, group discussion, and group decision-making, in which the stage of individual problem solving was a critical step but was often ignored. In this study, a new paper-based learning system integrated with digital materials was designed and implemented for enhancing face-to-face collaborative learning. The procedural scaffold was implemented using a smartphone. The results showed that the facilitation of the procedural scaffolding enabled groups to perform significantly better in resolving ill-structured problems, promoted higher-level discourse in group discussions, and fostered individuals¡¦ deep understanding. Relevant issues about student learning using the new system were discussed, and future research to improve this study was suggested.