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Knowledge payment is a new method of electronic learning that has developed in the era of social media. With the impact of the COVID-19 pandemic, the market for knowledge payment is rapidly expanding. Exploring the factors that influence users’ sustained willingness is beneficial for better communication between knowledge payment platforms and users, and for achieving a healthier and more sustainable development of the knowledge payment industry. The model of unsustainable usage behavior of knowledge payment users was constructed on the basis of expectation inconsistency theory, price equilibrium theory, and perceived value theory, using the “cognitive-emotional-behavioral” model framework of cognitive emotion theory. The data were collected from 348 users through a web-based questionnaire and analyzed using structural equation modeling. Findings show that expectation inconsistency, price equilibrium, and quality value, emotional value, and social value have significant effects on discontinuous use intentions. Discontinuous use intentions also significantly affect discontinuous use behavior.