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Problematic smartphone use can be defined as compulsive use that leads to impaired daily functioning in terms of productivity, social relationships, physical health, or emotional well-being. The current study provides a comprehensive assessment of how the broad and narrow traits of the HEXACO and Five Factor Models of personality predict problematic smartphone use. A sample of Australian adults (n = 393, 79% female; mean age = 24.4, SD = 7.1) completed the 300-item IPIP NEO and the 200-item HEXACO-PI-R, along with measures of general and problematic smartphone use. Participants reported high levels of problematic smartphone use. Problematic smartphone use was positively correlated with neuroticism and negatively correlated with conscientiousness. Facet-level analysis highlighted the importance of several facets including impulsiveness, vulnerability, and anxiety as positive correlates and dutifulness, competence, self-discipline, and deliberation as negative correlates of problematic smartphone use. In the HEXACO framework, honesty-humility, agreeableness, conscientiousness, and openness all showed moderate negative correlations with problematic smartphone use, and emotionality was positively correlated with problematic smartphone use. Regression models indicated that narrow traits provide modest incremental prediction of problematic use. Overall, the study highlights the importance of personality traits for understanding predispositions to engage in problematic smartphone use.