To deepen the teaching reform of physical chemistry experiments, an attempt has been made to enrich the physical chemistry experiments assisted by First Principle and Density Functional Theory calculations. In this paper, the simple and practical computational examples have been designed for the typical items of physical chemistry experiments. The calculation task includes steps such as building models, setting up parameters, submitting the calculation, analyzing the results. The application of the examples helps the students understand the relationship between the structure and properties of materials from a microscopic molecular level. The results indicate that most students are interested in doing chemical experiments on computer and they can complete the computational tasks. The comparison between the experimental and theoretical results helps the students understand the principles of physical chemistry. At the same time, it is favorable to train the students of their experimental and computational skills, which paves the way for scientific research for the future.