Despite the potential risks of excessive smartphone use for maladaptive outcomes, the link between smartphone use and aggression remains less understood. Furthermore, prior findings are inconclusive due to a narrow focus on limited aspects of smartphone use (e.g., screen time) and reliance on self-reported assessments of smartphone use. Therefore, using objective measures of smartphone use, we sought to examine the associations between several key indices of smartphone use—screen time, checking behaviors, and addictive tendency—and multifaceted aggression (i.e., confrontation, anger, and hostility). In a cross-sectional study, we administered a series of questionnaires assessing aggressive tendencies (i.e., The Aggression Questionnaire) and various aspects of smartphone use (N = 253, Mage = 21.8 years, female = 73.2%). Using structural equation modeling, we found that smartphone checking and addictive smartphone use predicted only hostility. In contrast, both objective and subjective measures of screen time did not predict any facets of aggression. These results highlight differing impacts of various indices of smartphone use on aggression and imply that excessive checking and addictive smartphone use are problematic smartphone-use behaviors that require more targeted interventions with respect to hostility.