As smartphones are emerging as a common device for adolescent, prior studies have provided theoretical and empirical evidence for the factors affecting adolescent smartphone use. However, mainstream research has tended to focus on the negative effects of smartphone. Even though smartphone use can have adverse outcomes, it may also allow students to engage in flexible mobile learning, gain access to important information about their possible future careers and achieve their personal goals. To fill this gap in adolescent smartphone usage, this study explored the smartphone usage patterns of adolescent subpopulations and the associations with their self-control, achievement goals, and academic achievements. Data were collected from 2341 s-year high school students as part of a larger longitudinal panel study. Three distinct smartphone usage profiles were identified in the latent profile analysis: learning, recreational use, and minimal use. Respondents with high perseverance were assigned to the learning group, and respondents with lower compliance and perseverance were assigned to the recreational group. The achievement goal score was found to be the highest in the learning group and lowest in the recreational group. Academic achievement was found to be higher in both the learning and minimal use groups than the recreational use group. Based on these findings, the implications of this study for research and practice are discussed.