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Although the terrestrial biosphere absorbs about 25 per cent of anthropogenic carbon dioxide (CO2) emissions, the rate of land carbon uptake remains highly uncertain, leading to uncertainties in climate projections(1,2). Understanding the factors that limit or drive land carbon storage is therefore important for improving climate predictions. One potential limiting factor for land carbon uptake is soil moisture, which can reduce gross primary production through ecosystem water stress(3,4), cause vegetation mortality(5) and further exacerbate climate extremes due to land-atmosphere feedbacks(6). Previous work has explored the impact of soil-moisture availability on past carbon-flux variability(3,7,8). However, the influence of soil-moisture variability and trends on the long-term carbon sink and the mechanisms responsible for associated carbon losses remain uncertain. Here we use the data output from four Earth system models(9) from a series of experiments to analyse the responses of terrestrial net biome productivity to soil-moisture changes, and find that soil-moisture variability and trends induce large CO2 fluxes (about two to three gigatons of carbon per year; comparable with the land carbon sink itself(1)) throughout the twenty-first century. Subseasonal and interannual soil-moisture variability generate CO2 as a result of the nonlinear response of photosynthesis and net ecosystem exchange to soil-water availability and of the increased temperature and vapour pressure deficit caused by land-atmosphere interactions. Soil-moisture variability reduces the present land carbon sink, and its increase and drying trends in several regions are expected to reduce it further. Our results emphasize that the capacity of continents to act as a future carbon sink critically depends on the nonlinear response of carbon fluxes to soil moisture and on land-atmosphere interactions. This suggests that the increasing trend in carbon uptake rate may not be sustained past the middle of the century and could result in accelerated atmospheric CO2 growth.