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This study aimed to empirically explore the relationship between destination attractiveness and tourists’ environmentally responsible behavior (TERB), as based on self-regulated attitude theory. In this paper, we have divided destination attractiveness into two aspects: the attractiveness of a facility’s services, and that of the sightseeing experience, so as to build a structural equation model with mediation analysis. For our research, we selected Wolong National Nature Reserve in Sichuan as the site of our case study, and we conducted a survey using a questionnaire. We then analyzed the path using a structural equation model. Our results show: (1) two elements of destination attractiveness have significantly positive effects on TERB; and (2) place attachment exerts a mediating effect among the attractiveness of the facility’s services, that of the sightseeing experience, and TERB. Therefore, enhancing destination attractiveness and tourists’ emotional attachments to locations could help to promote the implementation of TERB and the achievement of sustainable tourism development.