The work aims to study the influence of different atmosphere control methods on atmosphere evolution and corrosion of uranium assembly in uranium assembly storage containers, and obtain the optimized atmosphere control method. The method of virtual surface reaction was used to establish the calculation method of reaction between uranium material and environmental atmosphere, water release of organic materials and water absorption by desiccant. The humidity control and oxygen content in the container and the corrosion weight gain of uranium assembly were calculated under seven working conditions of separate use and combined use of such atmosphere control measures as improving the sealing performance of the container, drying agent and dispersion placement, drying agent treatment of organic material and so on. The effects of various atmosphere control measures were compared and analyzed. According to the research, only improving the sealing performance of the storage container containing uranium assembly would lead to anoxia in the container, thus accelerating the corrosion of uranium assembly. Desiccant placement was a better way to control the atmosphere, and the dispersion placement had a better effect. The atmosphere control measures of drying organic materials while dispersing desiccant had the best effect, as not only the corrosion rate of uranium assembly was the lowest, but also the state of aerobic low corrosion rate could be maintained for a long time. The evolution law of multi-component atmosphere in the storage container containing uranium assembly and the calculation method of corrosion change of uranium assembly are obtained. The effects of various atmosphere control methods on atmosphere control and reduction of corrosion of uranium assembly are compared and studied, and the optimized atmosphere control method is obtained.