Abstract: China has experienced a rapid land-use/cover change (LUCC) during the 20th Century, and this process is expected to continue in the future. How LUCC has affected water resources across China, however, remains uncertain due to the complexity of LUCC-water interactions. In this study, we used an integrated Dynamic Land Ecosystem Model (DLEM) in conjunction with spatial data of LUCC to estimate the LUCC effects on the magnitude, spatial and temporal variations of evapotranspiration (ET), runoff, and water yield across China. Through comparisons of DLEM results with other model simulations, field observations, and river discharge data, we found that DLEM model can adequately catch the spatial and seasonal patterns of hydrological processes. Our simulation results demonstrate that LUCC led to substantial changes in ET, runoff, and water yield in most of the China’s river basins during the 20th Century. The temporal and spatial patterns varied significantly across China. The largest change occurred during the second half century when almost all of the river basins had a decreasing trend in ET and an increasing trend in water yield and runoff, in contrast to the inclinations of ET and declinations of water yield in major river basins, such as Pearl river basin, Yangtze river basin, and Yellow river basin during the first half century. The increased water yield and runoff indicated alleviated water deficiency in China in the late 20th Century, but the increased peak flow might make the runoff difficult to be held by reservoirs. The continuously increasing ET and decreasing water yield in Continental river basin, Southwest river basin, and Songhua and Liaohe river basin implied regional water deficiency. Our study in China indicates that deforestation averagely increased ET by 138 mm/year but decreased water yield by the same amount and that reforestation averagely decreased ET by 422 mm/year since most of deforested land was converted to paddy land or irrigated cropland. In China, cropland-related land transformation is the dominant anthropogenic force affecting water resources during the 20th Century. On national average, cropland expansion was estimated to increase ET by 182 mm/year while cropland abandonment decreased ET by 379 mm/year. Our simulation results indicate that urban sprawl generally decreased ET and increased water yield. Cropland managements (fertilization and irrigation) significantly increased ET by 98 mm/year. To better understand LUCC effects on China’s water resources, it is needed to take into account the interactions of LUCC with other environmental changes such as climate and atmospheric composition.