There exists a complex relationship between cognition and behavior. Based on the characteristic that individuals have negative effects on the environment, this article defined the concept of undesired environmental behavior and explored the interaction effect of environmental context in the phenomenon of “disunity of cognition and behavior.” According to the survey data of Chinese residents, three main factors of the individual's environmental context were identified through factor analysis, including social norm, policy and regulation, and facilities support. The results of hierarchical linear regression show that: (1) Both environmental cognition and environmental context can significantly predict undesired environmental behavior, and social norm as well as facilities support can inhibit undesired environmental behavior except policy and regulation; (2) Undesired environmental behavior is affected by the interactions between environmental cognition and environmental context. Particularly, social norm and facilities support have influences on the relationship between environmental cognition and environmental context, and the relationship between the two is most influenced by facilities support. Finally, this article put forward related policy implications. © 2017 American Institute of Chemical Engineers Environ Prog, 37: 1361–1370, 2018