As the atmospheric carbon dioxide (CO2) increases substantially, the spatial distribution of atmospheric CO2 should be considered when estimating the effects of CO2 on the carbon and water cycle coupling of terrestrial ecosystems. To evaluate this effect on future ecohydrological processes, the spatial-temporal patterns of CO2 were established over 1951 - 2099 according to the IPCC emission scenarios SRES A2 and SRES B1. Thereafter, water use efficiency (WUE) was used (i.e., Net Primary Production/Evaportranspiration) as an indicator to quantify the effects of climate change and uneven CO2 fertilization in China. We carried out several simulated experiments to estimate WUE under different future scenarios using a land process model (Integrated Biosphere Simulator, IBIS). Results indicated that the geographical distributions of averaged WUE have considerable differences under a heterogeneous atmospheric CO2 condition. Under the SRES A2 scenario, WUE decreased slightly with a 5% value in most areas of the southeastern and northwestern China during the 2050s, while decreasing by approximately 15% in southeastern China during the 2090s. During the period of the 2050s under SRES B1 scenario, the change rate of WUE was similar with that under SRES A2 scenario, but the WUE has a more moderate decreasing trend than that under the SRES A2 scenario. In all, the ecosystems in median and low latitude areas had a weakened effect on resisting extreme climate event such as drought. Conversely, the vegetation in a boreal forest had an enhanced buffering capability to tolerate drought events.