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Knowledge sharing is an efficient method of enhancing teachers’ professional development. This study investigated the relationships among supervisor support (SS), teachers’ basic psychological needs satisfaction, trust in supervisors, and knowledge sharing behaviors, using data collected from 1522 primary and middle school teachers in China. We found SS had a positive impact on both knowledge donating and collecting. Teachers’ basic psychological needs satisfaction fully mediated the relationship between SS and teachers’ knowledge donating and partially mediated that between SS and knowledge collecting. Teachers’ trust in supervisors moderated the effects of SS on knowledge donating but not on knowledge collecting. The results also indicated that teachers’ trust in supervisors moderated the relationship between SS and teachers’ basic psychological needs satisfaction.