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Studies have been examining psychological factors or personal traits influential to individuals’ smartphone addiction; however, “self-regulation” and “self-regulated learning” have been neglected as a predictor variable of smartphone addiction. This study explores the interrelationship between Taiwanese college students’ self-regulation readiness and smartphone addiction. Results of this study should broaden our knowledge base regarding the antecedents of the smartphone addiction problem, based on which more holistic and granulated instructional or prevention strategies can be generated.