Rain use efficiency (RUE) quantifies the ecosystem's capacity to use precipitation water to assimilate atmospheric CO2. The spatial distribution of RUE and its drivers across the Australian continent is largely unknown. This knowledge gap limits our understanding of the possible contribution of Australian ecosystems to global carbon assimilation. This study investigates the spatial distribution of RUE across diverse terrestrial ecosystems in Australia. The results show that RUE ranges from 0.43 (1st percentile) to 3.10 (99th percentile) g C m−2 mm−1 with a continental mean of 1.19 g C m−2 mm−1. About 68 % of the spatiotemporal variability of RUE can be explained by a multiple linear regression model primarily contributed by climatic predictors. Benchmarked by the model estimation, drainage-diverging/converging landscapes tend to have reduced/increased RUE. The model also revealed the impact of increasing atmospheric CO2 concentration on RUE. The continental mean RUE would increase by between 29.3 and 64.8 % by the end of this century under the SSP5–8.5 scenario in which the CO2 concentration is projected to double from the present level. This increase in projected RUE is attributed to the assumed greening effect of increasing CO2 concentration, which does not consider the saturation of CO2 fertilisation effect and the warming effect on increasing wildfire occurrence. Under the SSP1–2.6 scenario, RUE would decrease by about 7 %. This study provides baseline RUEs of various ecosystems in Australia for investigating the impacts of human interferences and climate change on the capacity of Australian vegetation to assimilate atmospheric CO2 under given precipitation.