The interception of rainfall by vegetation canopies plays an important role in the hydrologic process of ecosystems. Most estimates of canopy rainfall interception in present studies are mainly through field observations at the plot region. However, it is difficult, yet important, to map the regional rainfall interception by vegetation canopy at a larger scale, especially in the southern rainy areas of China. To obtain a better understanding of the spatiotemporal variation of vegetation canopy rainfall interception with regard to the basin scale in this region, we extended a rainfall interception model by combining the observed rainfall data and moderate resolution imaging spectroradiometer leaf area index (MODIS_LAI) data to quantitatively estimate the vegetation canopy rainfall interception rate (CRIR) at small/medium basin scales in Guangdong Province, which is undergoing large changes in vegetation cover due to rapid urban expansion in the area. The results showed that the CRIR in Guangdong declined continuously during 2004-2012, but increased slightly in 2016, and the spatial variability of CRIR showed a diminishing yearly trend. The CRIR also exhibited a distinctive spatial pattern, with a higher rate to the east and west of the mountainous areas and a lower rate in the central mountainous and coastal areas. This pattern was more closely related to the spatial variation of the LAI than that of rainfall due to frequent extreme rainfall events saturating vegetation leaves. Further analysis demonstrated that forest coverage, instead of background climate, has a certain impact on the canopy rainfall interception, especially the proportion of broad-leaved forests in the basin, but more in-depth study is warranted in the future. In conclusion, the results of this study provide insights into the spatiotemporal variation of canopy rainfall interception at the basin scale of the Guangdong Province, and suggest that forest cover should be increased by adjusting the species composition to increase the proportion of native broad-leaved species based on the local condition within the basin. In addition, these results would be helpful in accurately assessing the impacts of forest ecosystems on regional water cycling, and provide scientific and practical implications for water resources management.