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The coach–athlete relationship influences an athlete’s psychological well-being; however, little is known about the psychological mechanisms involved in the relationship between these variables. This study emphasized the mediating role of psychological safety in the relationship between the coach–athlete relationship and athletes’ psychological well-being. Participants were 372 college athletes from five Chinese universities, who completed a paper-and-pencil questionnaire in which they assessed their coach–athlete relationship, psychological safety, and psychological well-being. Results of structural equation modeling indicated there was a positive relationship between a positive coach–athlete relationship and an athlete’s psychological well-being, and that psychological safety partially mediated this relationship. This study extends the conclusions of prior research and provides new insights into how the coach–athlete relationship affects athletes’ psychological well-being.