With the development of higher education and progress of the era, college students' subject consciousness gradually strengthens, and the colleges' work on constructing learning atmosphere is shifting from services to education by degrees. In this context, psychological contract spirit is proposed and applied to daily management of students. This paper briefly analyzes the fit of psychological contract spirit and construction of learning atmosphere among college students, and discusses the significance of psychological contract on the construction of colleges' learning atmosphere. It studies the strategy of constructing psychological contract for college students, and promotes the application and development of psychological contract spirit in the construction of colleges' learning atmosphere.