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Hundreds of millions of unstable croplands have been underutilized in the time series by repeated cultivation and abandonment, leading to threats to food security and loss of ecological benefits due to frequent disturbance on ecosystem restoration. Understanding unstable cropland and its connections to Sustainable Development Goals (SDGs) is required in the context of increasing food demand and natural conservation. Here, we first investigate the global cropland instability and influencing factors, then simulate the stable utilization of unstable cropland and its ecological effects under different scenarios of maintaining crop production. 395 million hectares of croplands in 173 countries are found under unstable utilization, accounting for 22% of global croplands. Over three-quarters of unstable croplands are distributed in areas with unfavorable agricultural conditions or high conservation value, and countries experiencing high cropland instability share a common characteristic of climatic or terrain constraints on agriculture. According to the simulation results, 141 million hectares or 36% of the unstable croplands could be released for ecological restoration with 3.8 more billion tons of carbon sequestration, while the rest of the unstable croplands could be stably used to increase 3% of global total crop production. This study highlights the importance of managing unstable croplands in climate mitigation and natural conservation as well as reconciling crop production and other SDGs, with guiding significance for land-use management, climate action, and biodiversity conservation. • 395 million hectares of croplands in 173 countries are under unstable utilization. • Three quarters of unstable croplands are constrained by natural and socio-economic factors. • 36% of the unstable croplands could be released for durable ecosystem recovery by simulation. • Projected increase of 3.8 billion tons of carbon sinks with a 3% increase in crop production. • Stabilizing unstable croplands can benefit the SDG win-win by lasting ecosystem recovery. [ABSTRACT FROM AUTHOR]