Identifying the spatial characteristics of ecosystem service (ES) supply and demand is crucial for effective ecosystem management and restoration. Past related studies have primarily focused on balancing ES supply and demand and supply clustering, with less attention focused on the drivers of demand clustering and their spatial evolution. This study explored the spatiotemporal supply–demand dynamics in four crucial ecosystem services (ESs) in the Sichuan-Yunnan ecological buffer area region between 2005 and 2019, namely water yield, net primary production, soil conservation, and habitat quality. Self-organizing maps and geographical detectors were used to classify supply–demand ES bundles as their main drivers, respectively. The main results of the study included: (1) A decline in habitat quality, whereas net primary productivity, water yield, and soil conservation increased. However, there were increasing demands for habitat quality, water yield, and net primary productivity, despite the decrease in demand for soil conservation. (2) Demand for habitat quality was met by supply, whereas there were deficits in soil conservation, water yield, and net primary productivity, which contributed to the demand in the east exceeding that elsewhere. (3) The proportion of ES bundle 2 increased, whereas those of the remaining ES bundles declined. Similarly, the areas of ES demand bundles (ESDBs) 1 and 4 decreased, whereas those of 2 and 3 increased. While the spatial extent of the ESBs remained relatively stable, those of the ESDBs in the northern regions increased. Key factors influencing the spatial distribution of ES supply include human activities, population density, and precipitation, whereas land use, population density, and the human activity index primarily affect demand distribution. The results of this study can act as a reference for comprehensive regional ecosystem management.