The purpose of this study is to explore the factors affecting college users’ willingness to participate in smart services of academic library. The paper analyzes the factors affecting college users’ willingness to participate in library smart services, and constructs a conceptual model with 17 hypotheses proposed, based on the theory of Uses and Gratifications, Social Cognition Theory, Innovation Diffusion Theory, and Information Systems Success Model. The conceptual model was empirically tested using structural equation modeling technique through questionnaire survey data. The questionnaire was distributed online to college students and teachers in different provinces of China by using random sampling technique. College users’ willingness to participate in smart services of academic library is directly and positively affected by information need of users, innovative consciousness of users, service platform performance, user satisfaction, library publicity and guidance, and extrinsic incentives. Information quality, service platform performance, service quality, and service value have significant and positive impact on user satisfaction, and they all indirectly affect users’ willingness to participate in smart services of academic library through user satisfaction. The survey results also show that the purpose of college students and teachers’ participation in smart services is mainly to meet their information needs. And users’ participation willingness is not affected by self-efficacy of users and others’ influence, which is different from the participation motivation of users on social Q & A and short video platforms. Understanding of factors affecting users’ willingness to participate in smart services of academic library will likely demand rethink into a number of issues ignored by studies on smart library and smart services. Few studies focus on users’ participation behavior in smart services of library. This study focused on the factors affecting users’ willingness to participate in smart services of academic library, which would expand the understanding of users’ participation behavior in smart services and enrich the scope of studies on smart library and smart services.