The article presents the results of a study of the development of mental regulation of students’ psychological states during their studies at a university. This work is based on authors’ conceptual model of the structural and functional organization of psychological states’ mental regulation. The study was carried out at the initial and final stages of students’ education in everyday and stressful situations of academic activity covering the period from 2019 to 2023. Methods and effectiveness of psychological state self-regulation were studied using well-known valid methods and specially designed questionnaires. Mental structures such as reflection, life meaning orientation, and self-system, as well as individual regulatory properties studied outside educational situations in first (2018) and fourth years (2022) of study were investigated. As a result of the study, it was established, that, regardless of the situation of educational activity, psychological states acquire greater stability (equilibrium) by the senior year of study, which is associated with the effectiveness of states’ self-regulation. Changes in mental structures from the initial course to the final of study are revealed in an increase in the intensity of their manifestations in all main indicators. It has been established that in both situations, during the learning process, students experience an increase in the involvement of mental structures (primarily reflexive) and regulatory properties in the regulation of psychological states. In each situation of educational activity and at each stage of training, there were identified the leading structures of consciousness, determining the choice of self-regulation methods, which, in turn, are associated with the substructures of psychological states. It has been also stablished that from the initial stage of study to the final one, there is an increase in the number of methods used for states’ self-regulation, as well as their relationships with mental structures and regulatory properties of the personality, which indicates the development of a system of mental regulation of students’ psychological states.