Investigating the relationship between factors (climate change, atmospheric CO₂ concentrations enrichment, and vegetation structure) and hydrological processes is important for understanding and predicting the interaction between the hydrosphere and biosphere. The Integrated Biosphere Simulator (IBIS) was used to evaluate the effects of climate change, rising CO₂, and vegetation structure on hydrological processes in China at the end of the 21st century. Seven simulations were implemented using the assemblage of the IPCC climate and CO₂ concentration scenarios, SRES A2 and SRES B1. Analysis results suggest that (1) climate change will have increasing effects on runoff, evapotranspiration (ET), transpiration (T), and transpiration ratio (transpiration/evapotranspiration, T/E) in most hydrological regions of China except in the southernmost regions; (2) elevated CO₂ concentrations will have increasing effects on runoff at the national scale, but at the hydrological region scale, the physiology effects induced by elevated CO₂ concentration will depend on the vegetation types, climate conditions, and geographical background information with noticeable decreasing effects shown in the arid Inland region of China; (3) leaf area index (LAI) compensation effect and stomatal closure effect are the dominant factors on runoff in the arid Inland region and southern moist hydrological regions, respectively; (4) the magnitudes of climate change (especially the changing precipitation pattern) effects on the water cycle are much larger than those of the elevated CO₂ concentration effects; however, increasing CO₂ concentration will be one of the most important modifiers to the water cycle; (5) the water resource condition will be improved in northern China but depressed in southernmost China under the IPCC climate change scenarios, SRES A2 and SRES B1.