The surface shortwave radiation budget (Rsn) is one of the main drivers of Earth’s ecosystems and varies with atmospheric and surface conditions. Land use and cover change (LUCC) alters radiation through biogeophysical effects. However, due to the complex interactions between atmospheric and surface factors, it is very challenging to quantify the sole impacts of LUCC. Based on satellite data from the Global Land Surface Satellite (GLASS) Product and Moderate Resolution Imaging Spectroradiometer (MODIS) instruments, this study introduces an observation-based approach for detecting LUCC influences on the Rsn by examining a humid basin over the Dongting Lake Basin, China from 2001 to 2015. Our results showed that the Rsn of the study area presented a decreasing trend due to the combined effects of LUCC and climate change. Generally, LUCC contributed −0.45 W/m² to Rsn at the basin scale, which accounted for 2.53% of the total Rsn change. Furthermore, the LUCC contributions reached −0.69 W/m², 0.21 W/m², and −0.41 W/m² in regions with land transitions of forest→grass, grass→forest, and grass→farmland, which accounted for 5.38%, −4.68%, and 2.40% of the total Rsn change, respectively. Physically, LUCC affected surface radiation by altering the surface properties. Specifically, LUCC induced albedo changes of +0.0039 at the basin scale and +0.0061, −0.0020, and +0.0036 in regions with land transitions of forest→grass, grass→forest, and grass→farmland, respectively. Our findings revealed the impact and process of LUCC on the surface radiation budget, which could support the understanding of the physical mechanisms of LUCC’s impact on ecosystems.