In this study, a one-year program was conducted to investigate the relationships between students' perceptions of mobile learning and their tendencies of peer interaction and higher-order thinking in issue-based mobile learning activities. To achieve the research objective, a survey consisting of eight scales, namely, usability, continuity, adaptive content, collaboration, communication, problem-solving, critical thinking and creativity, was developed. A total of 658 students from 38 high schools in Taiwan filled in the questionnaire after experiencing issue-based mobile learning activities. From the exploratory and confirmatory factor analyses, it was found that the questionnaire had high reliability and validity. The structural equation model further revealed that the provision of adaptive content in the mobile learning had positive impacts on the students' tendency to interact with peers (i.e., collaboration and communication), which further affected their tendency to engage in higher-order thinking (i.e., problem-solving, critical thinking, and creativity). The findings of this study provide a good reference for researchers and school teachers who intend to promote mobile learning in school settings.