Water is a prerequisite for the formation of earth-biochemical-ecological systems. Differences in the spatial and temporal distribution of water resources are important factors in the formation of differences in the distribution of vegetation in terrestrial ecosystems and are key to the differences in vegetation productivity. Vegetation water use efficiency is calculated by the total amount of fixed biogenic carbon per unit mass of water consumed in photosynthesis and can be used to assess the intensity and capacity of an ecosystem to use water biomass. Based on remote satellite sensing data, this study proposes a new water use efficiency assessment model. The model was validated using flux site data, and we analyzed the relative contribution of climate factors to soil moisture use efficiency using a first-difference method. The results revealed the following: (1) The soil moisture use efficiencies (SUE) of remote sensing data inversions that were evaluated using flux site data based on correlation coefficients and Nash coefficients showed high reliability, and only the NMG (Inner Mongolia) station showed low correlation among the nine sites. (2) Among the nine agricultural sub-regions in China, only the SUE of the Qinghai-Tibet Plateau region showed a decreasing trend (−1.08 g C/m−2 kg H2O yr), while all other regions showed an increasing trend. (3) The highest vegetation soil moisture use efficiency (1.83 g C/m−2 kg H2O) was found in ferralisols, while the lowest vegetation SUE (0.17 g C/m−2 kg H2O) was found in arid soils. The SUE of different vegetation types showed the characteristics of forest > scrub > cultivated vegetation > wetland > grassland. (4) The relative contribution of gross primary productivity (GPP) to the change in SUE was 37.53%, while the relative contribution of soil moisture content to the change in SUE was −26.71%. Among the five climatic factors, temperature was the most dominant factor affecting the change in SUE, followed by precipitation, net radiation, leaf area index, and potential evapotranspiration. Revealing the relationship between terrestrial ecosystem GPP, soil moisture content, and their responses to climate factors is a prerequisite for understanding the adaptation strategies of regional terrestrial ecosystems to global climate change, which can help to inform decision-making for the sustainable development of ecosystems.