With the rapid development of the general aviation industry in China, the influence of high-impact aeronautical weather events, such as aircraft icing, on flight safety has become more and more prominent. On 1 March 2021, an aircraft conducting weather modification operations crashed over Ji’an City, due to severe icing. Using multi-source meteorological observations and atmospheric numerical simulations, we analyzed the meteorological causes of this icing accident. The results indicate that a cold front formed in northwestern China and then moved southward, which is the main weather system in the icing area. Based on the icing index, we conducted an analysis of the temperature, relative humidity, cloud liquid water path, effective particle radius, and vertical flow field, it was found that aircraft icing occurred behind the ground front, where warm-moist airflows rose along the front to result in a rapid increase of water vapor in 600–500 hPa. The increase of water vapor, in conjunction with low temperature, led to the formation of a cold stratiform cloud system. In this cloud system, there were a large number of large cloud droplets. In addition, the frontal inversion increased the atmospheric stability, allowing cloud droplets to accumulate in the low-temperature region and forming meteorological conditions conducive to icing. The Weather Research and Forecasting model was employed to provide a detailed description of the formation process of the atmospheric conditions conducive to icing, such as the uplifting motion along the front and supercooled water. Based on a real case, we investigated the formation process of icing-inducing meteorological conditions under the influence of a front in detail in this study and verified the capability of a numerical model to simulate the meteorological environment of frontal icing, in order to provide a valuable reference for meteorological early warnings and forecasts for general aviation.