North China, characterized by its strong land–atmosphere coupling, also has a high concentration of atmospheric aerosols from anthropogenic emissions. However, the impact of aerosols on land–atmosphere coupling in this region remains partially unclear. Here, we use Weather Research and Forecasting model coupled with Chemistry (WRF‐Chem) experiments to show that the aerosol radiative effect weakens land–atmosphere coupling in North China. This weakening occurs across all five indexes used to measure different aspects of land–atmosphere coupling. Notably, the weakening is more pronounced for indexes that describe surface coupling compared to the index that characterizes the coupling between the planetary boundary layer (PBL) and clouds. The mechanisms underlying the aerosol influence can be primarily attributed to the reduction of land surface fluxes and their sensitivities to soil moisture, while the weakened entrainment of moisture at the upper boundary of the PBL may also contribute to the effects. Plain Language Summary The connection between land surface processes and atmospheric elements (land‐atmosphere coupling) is robust in North China due to its semi‐arid to semi‐humid climates. Additionally, the region experiences a high concentration of atmospheric pollution particles (aerosols) from human emissions. However, the impact of these aerosols on the land‐atmosphere coupling remains incompletely understood. To address this, we conducted experiments using a computer model. Our findings reveal that pollution weakens the land‐atmosphere coupling in North China. This effect is evident in various measures used to assess the coupling. Notably, the impact is more pronounced on the surface coupling compared to the coupling higher up in the atmosphere. The reasons behind this weakening effect are twofold. First, pollution reduces the exchange of heat and moisture between the land and the atmosphere. Second, it reduces the exchange of moisture in the upper atmosphere. Our research advances the understanding of land‐atmosphere interactions and their relationship with air pollution, potentially guiding future weather and climate predictions. Key Points Aerosol radiative effect weakens land–atmosphere coupling in North China, as found across five indexes of land–atmosphere coupling The weakening is more pronounced for surface coupling than the coupling between the planetary boundary layer and clouds The reduction of land surface fluxes and their sensitivities to soil moisture, along with the weakened entrainment are the primary mechanism