Background and Aim: This study adopts the teaching mode of self-regulated learning to change the traditional physical education teaching methods, so as to improve the physical literacy of college students. The component of college students' physical literacy includes physical cognition, physical experience, physical ability and sports behavior. The purpose of this study was to compare students' physical literacy scores before and after learning physical education course based on self-regulated learning. Materials and Methods: In this experimental study, 40 students (one class) from Zhoukou Normal University were investigated. This study used test and self-evaluation forms given to students before and after learning through physical education based on self-regulated learning. Data were collected and analyzed by means, standard deviation and t-test for dependent sample. Results: The results of the physical literacy before and after learning based on the self-regulated learning course, it was found that the mean scores of pretests of students' physical literacy were 188.88, SD was 25.45, and mean scores of posttests was 230.53, SD was 16.79. The post-test score of students' physical literacy was higher than that of the pre-test score, and the difference was statistically significance (t= 13.64, p<0.05). The average score of post-tests was progressively higher than the pre-test score. Conclusion: The developed physical education course based on self-regulated learning has a significant effect on improving the physical literacy of college students.