Rainwater harvesting could increase the resilience of ecosystems on the Loess Plateau and thus ensure the sustainability of livelihoods that depend on them. As such, it is a key component of strategies for adapting to global climate change. In this study, we used a new method to quantify the rainwater harvesting potential (RWHP) across the whole Loess Plateau and to characterize its spatial and temporal variation over the last four decades on the basis of the variable infiltration capacity model. It was found that that the mean RWHP of the study region was 731.10 × 108 m3, and the average water layer thickness was 114.34 mm. There is considerable scope for rainwater harvesting across the Loess Plateau as a whole, to the extent that it could potentially provide enough water to implement the ‘Grain for Green’ Project. The annual average RWHP decreased slightly from 1971 to 2010, and Hurst exponent analysis indicated that this trend will exhibit long-term persistence. The annual RWHP was highest in the southeast of the Loess Plateau and lowest in the northwest. Areas with high RWHP values tended to be clustered around the middle reach of the Yellow River. For most areas, there was no significant change between 1971 and 2010. Those areas for which there was a significant decrease in RWHP were primarily located around the upper–middle reaches of the Weihe River, the upper reach of Jinghe River, the eastern Guanzhong Plain, the Qinhe River watershed and the area around Dongsheng. Quantitative assessments of RWHP are likely to be useful for guiding the development and use of innovative rainwater harvesting technologies around the world and could help to relieve the problems caused by water shortages on the Loess Plateau while simultaneously eliminate the major cause of soil erosion. Copyright © 2012 John Wiley & Sons, Ltd.