This study aimed to investigate the potential bidirectionality between frustration of three basic needs (i.e., autonomy, relatedness, and competence) and problematic smartphone use (PSU), which is highly prevalent in adolescents. We recruited 466 Chinese high school students (61.6% female) for the baseline survey (W1), and 318 participated in the follow-up survey (W2). They completed questionnaires at both waves. Correlation analyses showed all three types of need frustration had significant positive associations with PSU at both waves. The cross-lagged panel model results supported the reciprocal relationship between autonomy frustration and PSU. PSU at W1 also predicted competence frustration at W2, whereas higher relatedness frustration levels at W1 predicted higher levels of autonomy/competence frustration at W2. Preventive programs for PSU would benefit from self-determination theory-based interventions that support a sense of autonomy and relatedness.