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The impacts of climate change on ecosystem productivity and water resources over a long term in China are not well quantified. Precipitation-use efficiency (PUE) is a key parameter that describes carbon and water exchange in terrestrial ecosystems. Research on the response of regional PUE to climate change and its driving forces is of great significance to climate-change mitigation and the sustainable development of regional ecology. Based on an improved actual evapotranspiration (ET_a) model, the responses of ET_a, net primary productivity (NPP), and PUE to climate change in different climatic regions of China were analyzed; the contributions of various environmental factors to PUE changes were quantified; and the conversion characteristics and regulatory mechanisms of the PUE regime in different climatic regions were identified. The results indicate that the improved ET_a model, after considering the limiting effect of energy on ET_a in humid regions, can simulate the ET_a distribution in China well. Over the past 58 years (1960–2017), ET_a and NPP have increased in the western regions and decreased in the eastern regions, with the boundary at 103° E. PUE presents a “low-high-low” spatial distribution from northwest to southeast in China. It is noteworthy that there was a zonal distribution for a high value area of PUE, which coincided with the summer monsoon transition zone. The soil moisture (SM) increase in arid regions is the main driving force of the PUE increase, whereas the annual net radiation (Rn) change in humid regions is the main driving force of the PUE change. The transition zone is the conversion zone, where the prevailing factor limiting vegetation growth transitions from water to energy.