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We examined whether autonomy satisfaction and frustration could be empirically distinguished and had different predictive relationships with students’ academic motivation and achievement in math and English. Results based on a group of 3142 Chinese adolescent students revealed that autonomy satisfaction and frustration were two distinguishable constructs and demonstrated distinct predictive utility. In specific, autonomy satisfaction significantly predicted self-efficacy, which in turn leads to higher achievement. Autonomy satisfaction also significantly predicted interest value. In contrast, autonomy frustration significantly predicted effort cost, which subsequently undermines achievement. Furthermore, these patterns were highly consistent across two subject domains. Findings of the present study highlight the importance of differentiating autonomy satisfaction and frustration when predicting students’ educational outcomes.