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We examined whether relatedness satisfaction and frustration could be empirically distinguished and had different predictive relationships with students’ academic outcomes and school burnout. Results based on a group of 1639 Chinese adolescent students revealed that relatedness satisfaction and frustration were two distinguishable constructs and demonstrated distinct predictive utility. In specific, relatedness satisfaction significantly predicted persistence, which in turn leads to higher achievement. In contrast, relatedness frustration significantly predicted procrastination, which leads to higher school burnout. Relatedness frustration also significantly predicted school burnout directly. Findings of the present study highlight the importance of differentiating relatedness satisfaction and frustration when predicting students’ academic functioning.